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1374 |
> |
y Fn(1{3)1373 3706 y Fu(Man)n(y)g(of)h(these)-150 3801 |
1375 |
|
y(mo)r(dels)22 b(get)g(sp)r(eci\014c)g(prop)r(erties)f(correct)f(or)h |
1376 |
< |
(b)r(etter)h(than)g(their)-150 3891 y(predecessors,)38 |
1376 |
> |
(b)r(etter)h(than)g(their)-150 3897 y(predecessors,)38 |
1377 |
|
b(but)h(this)f(is)g(often)g(at)g(a)f(cost)h(of)g(some)f(other)-150 |
1378 |
< |
3987 y(prop)r(erties)g(or)g(of)g(computer)g(time.)68 |
1379 |
< |
b(As)38 b(an)f(example,)j(com-)-150 4082 y(pare)27 b(TIP3P)f(or)h |
1378 |
> |
3992 y(prop)r(erties)g(or)g(of)g(computer)g(time.)68 |
1379 |
> |
b(As)38 b(an)f(example,)j(com-)-150 4088 y(pare)27 b(TIP3P)f(or)h |
1380 |
|
(TIP4P)f(to)h(TIP5P)-7 b(.)26 b(TIP5P)h(succeeds)g(in)g(im-)-150 |
1381 |
< |
4178 y(pro)n(ving)j(the)j(structural)e(and)g(transp)r(ort)g(prop)r |
1382 |
< |
(erties)g(o)n(v)n(er)f(its)-150 4273 y(predecessors,)36 |
1381 |
> |
4183 y(pro)n(ving)j(the)j(structural)e(and)g(transp)r(ort)g(prop)r |
1382 |
> |
(erties)g(o)n(v)n(er)f(its)-150 4279 y(predecessors,)36 |
1383 |
|
b(y)n(et)g(this)g(comes)g(at)g(a)f(greater)g(than)h(50\045)f(in-)-150 |
1384 |
< |
4369 y(crease)30 b(in)h(computational)g(cost.)919 4339 |
1385 |
< |
y Fn(3)o(,4)1039 4369 y Fu(One)f(recen)n(tly)h(dev)n(elop)r(ed)-150 |
1386 |
< |
4464 y(mo)r(del)36 b(that)g(succeeds)f(in)g(b)r(oth)h(retaining)f |
1387 |
< |
(accuracy)f(of)h(sys-)-150 4560 y(tem)j(prop)r(erties)e(and)i |
1388 |
< |
(simplifying)f(calculations)f(to)i(increase)-150 4655 |
1384 |
> |
4374 y(crease)30 b(in)h(computational)g(cost.)919 4344 |
1385 |
> |
y Fn(3)o(,4)1039 4374 y Fu(One)f(recen)n(tly)h(dev)n(elop)r(ed)-150 |
1386 |
> |
4470 y(mo)r(del)36 b(that)g(succeeds)f(in)g(b)r(oth)h(retaining)f |
1387 |
> |
(accuracy)f(of)h(sys-)-150 4565 y(tem)j(prop)r(erties)e(and)i |
1388 |
> |
(simplifying)f(calculations)f(to)i(increase)-150 4661 |
1389 |
|
y(computational)30 b(e\016ciency)g(is)h(the)f(Soft)h(Stic)n(ky)g(Dip)r |
1390 |
< |
(ole)f(w)n(ater)-150 4751 y(mo)r(del.)92 4720 y Fn(5)-67 |
1391 |
< |
4846 y Fu(The)e(Soft)h(Stic)n(ky)f(Dip)r(ole)h(\(SSD\))g(w)n(ater)f(mo) |
1392 |
< |
r(del)g(w)n(as)f(dev)n(el-)-150 4942 y(op)r(ed)37 b(b)n(y)h(Ic)n(hiy)n |
1390 |
> |
(ole)f(w)n(ater)-150 4756 y(mo)r(del.)92 4726 y Fn(5)-67 |
1391 |
> |
4852 y Fu(The)e(Soft)h(Stic)n(ky)f(Dip)r(ole)h(\(SSD\))g(w)n(ater)f(mo) |
1392 |
> |
r(del)g(w)n(as)f(dev)n(el-)-150 4947 y(op)r(ed)37 b(b)n(y)h(Ic)n(hiy)n |
1393 |
|
(e)e Fm(et)j(al.)67 b Fu(as)37 b(a)g(mo)r(di\014ed)h(form)f(of)h(the)f |
1394 |
< |
(hard-)-150 5037 y(sphere)48 b(w)n(ater)g(mo)r(del)h(prop)r(osed)e(b)n |
1395 |
< |
(y)i(Bratk)n(o,)j(Blum,)j(and)p -150 5206 300 4 v -59 |
1396 |
< |
5384 a Fl(\003)-23 5407 y Fk(Corresp)r(onding)24 b(author.)55 |
1397 |
< |
b(Electronic)25 b(mail:)k(gezelter@nd.edu)2042 2150 y |
1398 |
< |
Fu(Luzar.)2275 2120 y Fn(6)o(,7)2403 2150 y Fu(SSD)42 |
1394 |
> |
(hard-)-150 5043 y(sphere)48 b(w)n(ater)g(mo)r(del)h(prop)r(osed)e(b)n |
1395 |
> |
(y)i(Bratk)n(o,)j(Blum,)j(and)p -150 5212 300 4 v -59 |
1396 |
> |
5390 a Fl(\003)-23 5413 y Fk(Corresp)r(onding)24 b(author.)55 |
1397 |
> |
b(Electronic)25 b(mail:)k(gezelter@nd.edu)2042 2156 y |
1398 |
> |
Fu(Luzar.)2275 2126 y Fn(6)o(,7)2403 2156 y Fu(SSD)42 |
1399 |
|
b(consists)d(of)i(a)f(single)f(p)r(oin)n(t)i(dip)r(ole)g(with)g(a)2042 |
1400 |
< |
2246 y(Lennard-Jones)35 b(core)i(and)h(a)f(stic)n(ky)g(p)r(oten)n(tial) |
1401 |
< |
h(that)g(directs)2042 2341 y(the)27 b(particles)f(to)g(assume)g(the)h |
1402 |
< |
(prop)r(er)e(h)n(ydrogen)g(b)r(ond)i(orien-)2042 2437 |
1400 |
> |
2251 y(Lennard-Jones)35 b(core)i(and)h(a)f(stic)n(ky)g(p)r(oten)n(tial) |
1401 |
> |
h(that)g(directs)2042 2347 y(the)27 b(particles)f(to)g(assume)g(the)h |
1402 |
> |
(prop)r(er)e(h)n(ydrogen)g(b)r(ond)i(orien-)2042 2442 |
1403 |
|
y(tation)32 b(in)h(the)g(\014rst)f(solv)-5 b(ation)31 |
1404 |
|
b(shell.)52 b(Th)n(us,)33 b(the)g(in)n(teraction)2042 |
1405 |
< |
2532 y(b)r(et)n(w)n(een)24 b(t)n(w)n(o)f(SSD)i(w)n(ater)d(molecules)i |
1405 |
> |
2538 y(b)r(et)n(w)n(een)24 b(t)n(w)n(o)f(SSD)i(w)n(ater)d(molecules)i |
1406 |
|
Fm(i)33 b Fu(and)24 b Fm(j)36 b Fu(is)24 b(giv)n(en)f(b)n(y)h(the)2042 |
1407 |
< |
2628 y(p)r(oten)n(tial)2083 2815 y Fj(u)2131 2827 y Fi(ij)2212 |
1408 |
< |
2815 y Fu(=)f Fj(u)2348 2781 y Fi(LJ)2348 2836 y(ij)2439 |
1409 |
< |
2815 y Fu(\()p Fj(r)2508 2827 y Fi(ij)2568 2815 y Fu(\))29 |
1410 |
< |
b(+)7 b Fj(u)2749 2775 y Fi(dp)2749 2838 y(ij)2822 2815 |
1411 |
< |
y Fu(\()p Fh(r)2893 2827 y Fi(ij)2952 2815 y Fj(;)14 |
1412 |
< |
b Fh(\012)3058 2827 y Fi(i)3085 2815 y Fj(;)g Fh(\012)3191 |
1413 |
< |
2827 y Fi(j)3226 2815 y Fu(\))30 b(+)7 b Fj(u)3408 2775 |
1414 |
< |
y Fi(sp)3408 2838 y(ij)3477 2815 y Fu(\()p Fh(r)3548 |
1415 |
< |
2827 y Fi(ij)3607 2815 y Fj(;)14 b Fh(\012)3713 2827 |
1416 |
< |
y Fi(i)3740 2815 y Fj(;)g Fh(\012)3846 2827 y Fi(j)3881 |
1417 |
< |
2815 y Fu(\))p Fj(;)42 b Fu(\(1\))2042 2994 y(where)36 |
1418 |
< |
b(the)i Fh(r)2483 3006 y Fi(ij)2578 2994 y Fu(is)f(the)g(p)r(osition)g |
1419 |
< |
(v)n(ector)f(b)r(et)n(w)n(een)h(molecules)2042 3089 y |
1407 |
> |
2633 y(p)r(oten)n(tial)2083 2821 y Fj(u)2131 2833 y Fi(ij)2212 |
1408 |
> |
2821 y Fu(=)f Fj(u)2348 2787 y Fi(LJ)2348 2841 y(ij)2439 |
1409 |
> |
2821 y Fu(\()p Fj(r)2508 2833 y Fi(ij)2568 2821 y Fu(\))29 |
1410 |
> |
b(+)7 b Fj(u)2749 2781 y Fi(dp)2749 2844 y(ij)2822 2821 |
1411 |
> |
y Fu(\()p Fh(r)2893 2833 y Fi(ij)2952 2821 y Fj(;)14 |
1412 |
> |
b Fh(\012)3058 2833 y Fi(i)3085 2821 y Fj(;)g Fh(\012)3191 |
1413 |
> |
2833 y Fi(j)3226 2821 y Fu(\))30 b(+)7 b Fj(u)3408 2781 |
1414 |
> |
y Fi(sp)3408 2844 y(ij)3477 2821 y Fu(\()p Fh(r)3548 |
1415 |
> |
2833 y Fi(ij)3607 2821 y Fj(;)14 b Fh(\012)3713 2833 |
1416 |
> |
y Fi(i)3740 2821 y Fj(;)g Fh(\012)3846 2833 y Fi(j)3881 |
1417 |
> |
2821 y Fu(\))p Fj(;)42 b Fu(\(1\))2042 2999 y(where)36 |
1418 |
> |
b(the)i Fh(r)2483 3011 y Fi(ij)2578 2999 y Fu(is)f(the)g(p)r(osition)g |
1419 |
> |
(v)n(ector)f(b)r(et)n(w)n(een)h(molecules)2042 3095 y |
1420 |
|
Fm(i)44 b Fu(and)35 b Fm(j)48 b Fu(with)36 b(magnitude)f(equal)g(to)g |
1421 |
< |
(the)h(distance)f Fj(r)3823 3101 y Fi(i)3851 3089 y Fj(j)5 |
1422 |
< |
b Fu(,)37 b(and)2042 3185 y Fh(\012)2111 3197 y Fi(i)2175 |
1423 |
< |
3185 y Fu(and)g Fh(\012)2415 3197 y Fi(j)2486 3185 y |
1421 |
> |
(the)h(distance)f Fj(r)3823 3107 y Fi(i)3851 3095 y Fj(j)5 |
1422 |
> |
b Fu(,)37 b(and)2042 3190 y Fh(\012)2111 3202 y Fi(i)2175 |
1423 |
> |
3190 y Fu(and)g Fh(\012)2415 3202 y Fi(j)2486 3190 y |
1424 |
|
Fu(represen)n(t)f(the)h(orien)n(tations)e(of)i(the)g(resp)r(ectiv)n(e) |
1425 |
< |
2042 3280 y(molecules.)47 b(The)32 b(Lennard-Jones,)e(dip)r(ole,)i(and) |
1426 |
< |
f(stic)n(ky)g(parts)2042 3376 y(of)c(the)h(p)r(oten)n(tial)g(are)e |
1425 |
> |
2042 3286 y(molecules.)47 b(The)32 b(Lennard-Jones,)e(dip)r(ole,)i(and) |
1426 |
> |
f(stic)n(ky)g(parts)2042 3381 y(of)c(the)h(p)r(oten)n(tial)g(are)e |
1427 |
|
(giving)h(b)n(y)h(the)g(follo)n(wing)e(equations,)2404 |
1428 |
< |
3628 y Fj(u)2452 3594 y Fi(LJ)2452 3649 y(ij)2543 3628 |
1429 |
< |
y Fu(\()p Fj(r)2612 3640 y Fi(ij)2671 3628 y Fu(\))e(=)e(4)p |
1430 |
< |
Fj(\017)2904 3486 y Fg(")2952 3511 y(\022)3046 3572 y |
1431 |
< |
Fj(\033)p 3023 3609 96 4 v 3023 3685 a(r)3060 3697 y |
1432 |
< |
Fi(ij)3129 3511 y Fg(\023)3190 3529 y Fn(12)3279 3628 |
1433 |
< |
y Ff(\000)3362 3511 y Fg(\022)3455 3572 y Fj(\033)p 3433 |
1434 |
< |
3609 V 3433 3685 a(r)3470 3697 y Fi(ij)3539 3511 y Fg(\023)3600 |
1435 |
< |
3529 y Fn(6)3637 3486 y Fg(#)3699 3628 y Fj(;)256 b Fu(\(2\))2398 |
1436 |
< |
4033 y Fj(u)2446 3993 y Fi(dp)2446 4056 y(ij)2542 4033 |
1437 |
< |
y Fu(=)2639 3969 y Fe(\026)2698 3989 y Fi(i)2744 3969 |
1438 |
< |
y Ff(\001)19 b Fe(\026)2844 3989 y Fi(j)p 2639 4014 241 |
1439 |
< |
4 v 2711 4090 a Fj(r)2750 4061 y Fn(3)2748 4113 y Fi(ij)2908 |
1440 |
< |
4033 y Ff(\000)3001 3969 y Fu(3\()p Fe(\026)3133 3989 |
1441 |
< |
y Fi(i)3179 3969 y Ff(\001)g Fh(r)3260 3981 y Fi(ij)3319 |
1442 |
< |
3969 y Fu(\)\()p Fe(\026)3442 3989 y Fi(j)3495 3969 y |
1443 |
< |
Ff(\001)g Fh(r)3576 3981 y Fi(ij)3635 3969 y Fu(\))p |
1444 |
< |
3001 4014 667 4 v 3286 4090 a Fj(r)3325 4061 y Fn(5)3323 |
1445 |
< |
4113 y Fi(ij)3705 4033 y Fj(;)250 b Fu(\(3\))2271 4390 |
1446 |
< |
y Fj(u)2319 4351 y Fi(sp)2319 4414 y(ij)2388 4390 y Fu(\()p |
1447 |
< |
Fh(r)2459 4402 y Fi(ij)2518 4390 y Fj(;)14 b Fh(\012)2624 |
1448 |
< |
4402 y Fi(i)2652 4390 y Fj(;)g Fh(\012)2757 4402 y Fi(j)2792 |
1449 |
< |
4390 y Fu(\))24 b(=)2945 4334 y Fj(\027)2986 4346 y Fn(0)p |
1450 |
< |
2945 4371 79 4 v 2964 4447 a Fu(2)3034 4390 y([)p Fj(s)p |
1451 |
< |
Fu(\()p Fj(r)3165 4402 y Fi(ij)3224 4390 y Fu(\))p Fj(w)r |
1452 |
< |
Fu(\()p Fh(r)3388 4402 y Fi(ij)3448 4390 y Fj(;)14 b |
1453 |
< |
Fh(\012)3554 4402 y Fi(i)3581 4390 y Fj(;)g Fh(\012)3687 |
1454 |
< |
4402 y Fi(j)3722 4390 y Fu(\))2954 4547 y(+)k Fj(s)3076 |
1455 |
< |
4513 y Ft(0)3099 4547 y Fu(\()p Fj(r)3168 4559 y Fi(ij)3227 |
1456 |
< |
4547 y Fu(\))p Fj(w)3320 4513 y Ft(0)3345 4547 y Fu(\()p |
1457 |
< |
Fh(r)3416 4559 y Fi(ij)3475 4547 y Fj(;)c Fh(\012)3581 |
1458 |
< |
4559 y Fi(i)3608 4547 y Fj(;)g Fh(\012)3714 4559 y Fi(j)3749 |
1459 |
< |
4547 y Fu(\)])28 b Fj(;)3978 4458 y Fu(\(4\))2042 4725 |
1460 |
< |
y(where)h Fe(\026)2343 4745 y Fi(i)2400 4725 y Fu(and)g |
1461 |
< |
Fe(\026)2622 4745 y Fi(j)2687 4725 y Fu(are)f(the)i(dip)r(ole)g(unit)g |
1462 |
< |
(v)n(ectors)e(of)i(particles)2042 4821 y Fm(i)35 b Fu(and)27 |
1428 |
> |
3634 y Fj(u)2452 3600 y Fi(LJ)2452 3654 y(ij)2543 3634 |
1429 |
> |
y Fu(\()p Fj(r)2612 3646 y Fi(ij)2671 3634 y Fu(\))e(=)e(4)p |
1430 |
> |
Fj(\017)2904 3492 y Fg(")2952 3517 y(\022)3046 3578 y |
1431 |
> |
Fj(\033)p 3023 3615 96 4 v 3023 3691 a(r)3060 3703 y |
1432 |
> |
Fi(ij)3129 3517 y Fg(\023)3190 3534 y Fn(12)3279 3634 |
1433 |
> |
y Ff(\000)3362 3517 y Fg(\022)3455 3578 y Fj(\033)p 3433 |
1434 |
> |
3615 V 3433 3691 a(r)3470 3703 y Fi(ij)3539 3517 y Fg(\023)3600 |
1435 |
> |
3534 y Fn(6)3637 3492 y Fg(#)3699 3634 y Fj(;)256 b Fu(\(2\))2398 |
1436 |
> |
4038 y Fj(u)2446 3998 y Fi(dp)2446 4061 y(ij)2542 4038 |
1437 |
> |
y Fu(=)2639 3974 y Fe(\026)2698 3995 y Fi(i)2744 3974 |
1438 |
> |
y Ff(\001)19 b Fe(\026)2844 3995 y Fi(j)p 2639 4019 241 |
1439 |
> |
4 v 2711 4095 a Fj(r)2750 4067 y Fn(3)2748 4118 y Fi(ij)2908 |
1440 |
> |
4038 y Ff(\000)3001 3974 y Fu(3\()p Fe(\026)3133 3995 |
1441 |
> |
y Fi(i)3179 3974 y Ff(\001)g Fh(r)3260 3986 y Fi(ij)3319 |
1442 |
> |
3974 y Fu(\)\()p Fe(\026)3442 3995 y Fi(j)3495 3974 y |
1443 |
> |
Ff(\001)g Fh(r)3576 3986 y Fi(ij)3635 3974 y Fu(\))p |
1444 |
> |
3001 4019 667 4 v 3286 4095 a Fj(r)3325 4067 y Fn(5)3323 |
1445 |
> |
4118 y Fi(ij)3705 4038 y Fj(;)250 b Fu(\(3\))2271 4396 |
1446 |
> |
y Fj(u)2319 4356 y Fi(sp)2319 4419 y(ij)2388 4396 y Fu(\()p |
1447 |
> |
Fh(r)2459 4408 y Fi(ij)2518 4396 y Fj(;)14 b Fh(\012)2624 |
1448 |
> |
4408 y Fi(i)2652 4396 y Fj(;)g Fh(\012)2757 4408 y Fi(j)2792 |
1449 |
> |
4396 y Fu(\))24 b(=)2945 4340 y Fj(\027)2986 4352 y Fn(0)p |
1450 |
> |
2945 4377 79 4 v 2964 4453 a Fu(2)3034 4396 y([)p Fj(s)p |
1451 |
> |
Fu(\()p Fj(r)3165 4408 y Fi(ij)3224 4396 y Fu(\))p Fj(w)r |
1452 |
> |
Fu(\()p Fh(r)3388 4408 y Fi(ij)3448 4396 y Fj(;)14 b |
1453 |
> |
Fh(\012)3554 4408 y Fi(i)3581 4396 y Fj(;)g Fh(\012)3687 |
1454 |
> |
4408 y Fi(j)3722 4396 y Fu(\))2954 4553 y(+)k Fj(s)3076 |
1455 |
> |
4519 y Ft(0)3099 4553 y Fu(\()p Fj(r)3168 4565 y Fi(ij)3227 |
1456 |
> |
4553 y Fu(\))p Fj(w)3320 4519 y Ft(0)3345 4553 y Fu(\()p |
1457 |
> |
Fh(r)3416 4565 y Fi(ij)3475 4553 y Fj(;)c Fh(\012)3581 |
1458 |
> |
4565 y Fi(i)3608 4553 y Fj(;)g Fh(\012)3714 4565 y Fi(j)3749 |
1459 |
> |
4553 y Fu(\)])28 b Fj(;)3978 4464 y Fu(\(4\))2042 4731 |
1460 |
> |
y(where)h Fe(\026)2343 4751 y Fi(i)2400 4731 y Fu(and)g |
1461 |
> |
Fe(\026)2622 4751 y Fi(j)2687 4731 y Fu(are)f(the)i(dip)r(ole)g(unit)g |
1462 |
> |
(v)n(ectors)e(of)i(particles)2042 4826 y Fm(i)35 b Fu(and)27 |
1463 |
|
b Fm(j)39 b Fu(with)27 b(magnitude)g(2.35)e(D,)i Fj(\027)3253 |
1464 |
< |
4833 y Fn(0)3317 4821 y Fu(scales)f(the)h(strength)f(of)2042 |
1465 |
< |
4916 y(the)j(o)n(v)n(erall)d(stic)n(ky)i(p)r(oten)n(tial,)h |
1466 |
< |
Fj(s)g Fu(and)f Fj(s)3335 4886 y Ft(0)3387 4916 y Fu(are)g(cubic)h |
1467 |
< |
(switc)n(hing)2042 5011 y(functions.)71 b(The)39 b Fj(w)j |
1468 |
< |
Fu(and)d Fj(w)2983 4981 y Ft(0)3046 5011 y Fu(functions)h(tak)n(e)e |
1469 |
< |
(the)h(follo)n(wing)2042 5107 y(forms,)2362 5285 y Fj(w)r |
1470 |
< |
Fu(\()p Fh(r)2494 5297 y Fi(ij)2554 5285 y Fj(;)14 b |
1471 |
< |
Fh(\012)2659 5297 y Fi(i)2687 5285 y Fj(;)g Fh(\012)2793 |
1472 |
< |
5297 y Fi(j)2828 5285 y Fu(\))23 b(=)g(sin)14 b Fj(\022)3126 |
1473 |
< |
5297 y Fi(ij)3198 5285 y Fu(sin)g(2)p Fj(\022)3395 5297 |
1474 |
< |
y Fi(ij)3467 5285 y Fu(cos)f(2)p Fj(\036)3683 5297 y |
1475 |
< |
Fi(ij)3741 5285 y Fj(;)214 b Fu(\(5\))2083 5555 y Fj(w)2144 |
1476 |
< |
5521 y Ft(0)2168 5555 y Fu(\()p Fh(r)2239 5567 y Fi(ij)2298 |
1477 |
< |
5555 y Fj(;)14 b Fh(\012)2404 5567 y Fi(i)2432 5555 y |
1478 |
< |
Fj(;)g Fh(\012)2538 5567 y Fi(j)2573 5555 y Fu(\))23 |
1479 |
< |
b(=)g(\(cos)13 b Fj(\022)2912 5567 y Fi(ij)2978 5555 |
1480 |
< |
y Ff(\000)7 b Fu(0)p Fj(:)p Fu(6\))3189 5521 y Fn(2)3225 |
1481 |
< |
5555 y Fu(\(cos)14 b Fj(\022)3422 5567 y Fi(ij)3488 5555 |
1482 |
< |
y Fu(+)7 b(0)p Fj(:)p Fu(8\))3699 5521 y Fn(2)3743 5555 |
1483 |
< |
y Ff(\000)g Fj(w)3876 5521 y Fn(0)3913 5555 y Fj(;)42 |
1464 |
> |
4838 y Fn(0)3317 4826 y Fu(scales)f(the)h(strength)f(of)2042 |
1465 |
> |
4922 y(the)j(o)n(v)n(erall)d(stic)n(ky)i(p)r(oten)n(tial,)h |
1466 |
> |
Fj(s)g Fu(and)f Fj(s)3335 4891 y Ft(0)3387 4922 y Fu(are)g(cubic)h |
1467 |
> |
(switc)n(hing)2042 5017 y(functions.)71 b(The)39 b Fj(w)j |
1468 |
> |
Fu(and)d Fj(w)2983 4987 y Ft(0)3046 5017 y Fu(functions)h(tak)n(e)e |
1469 |
> |
(the)h(follo)n(wing)2042 5112 y(forms,)2362 5291 y Fj(w)r |
1470 |
> |
Fu(\()p Fh(r)2494 5303 y Fi(ij)2554 5291 y Fj(;)14 b |
1471 |
> |
Fh(\012)2659 5303 y Fi(i)2687 5291 y Fj(;)g Fh(\012)2793 |
1472 |
> |
5303 y Fi(j)2828 5291 y Fu(\))23 b(=)g(sin)14 b Fj(\022)3126 |
1473 |
> |
5303 y Fi(ij)3198 5291 y Fu(sin)g(2)p Fj(\022)3395 5303 |
1474 |
> |
y Fi(ij)3467 5291 y Fu(cos)f(2)p Fj(\036)3683 5303 y |
1475 |
> |
Fi(ij)3741 5291 y Fj(;)214 b Fu(\(5\))2083 5561 y Fj(w)2144 |
1476 |
> |
5527 y Ft(0)2168 5561 y Fu(\()p Fh(r)2239 5573 y Fi(ij)2298 |
1477 |
> |
5561 y Fj(;)14 b Fh(\012)2404 5573 y Fi(i)2432 5561 y |
1478 |
> |
Fj(;)g Fh(\012)2538 5573 y Fi(j)2573 5561 y Fu(\))23 |
1479 |
> |
b(=)g(\(cos)13 b Fj(\022)2912 5573 y Fi(ij)2978 5561 |
1480 |
> |
y Ff(\000)7 b Fu(0)p Fj(:)p Fu(6\))3189 5527 y Fn(2)3225 |
1481 |
> |
5561 y Fu(\(cos)14 b Fj(\022)3422 5573 y Fi(ij)3488 5561 |
1482 |
> |
y Fu(+)7 b(0)p Fj(:)p Fu(8\))3699 5527 y Fn(2)3743 5561 |
1483 |
> |
y Ff(\000)g Fj(w)3876 5527 y Fn(0)3913 5561 y Fj(;)42 |
1484 |
|
b Fu(\(6\))p eop |
1485 |
|
%%Page: 2 2 |
1486 |
|
2 1 bop 4043 -299 a Fu(2)-150 -83 y(where)31 b Fj(w)155 |
1504 |
|
(del,)h(Ic)n(hiy)n(e)-150 872 y Fm(et)31 b(al.)45 b Fu(rep)r(orted)29 |
1505 |
|
b(a)g(calculation)g(sp)r(eed)h(up)g(of)g(up)g(to)f(an)h(order)-150 |
1506 |
|
967 y(of)d(magnitude)g(o)n(v)n(er)e(other)h(comparable)g(mo)r(dels)h |
1507 |
< |
(while)g(main-)-150 1063 y(taining)f(the)h(structural)f(b)r(eha)n(vior) |
1508 |
< |
g(of)g(w)n(ater.)1312 1033 y Fn(5)1375 1063 y Fu(In)h(the)g(original) |
1509 |
< |
-150 1158 y(molecular)35 b(dynamics)h(studies)h(of)g(SSD,)g(it)g(w)n |
1510 |
< |
(as)e(sho)n(wn)h(that)-150 1254 y(it)f(actually)e(impro)n(v)n(es)g(up)r |
1511 |
< |
(on)h(the)h(prediction)f(of)g(w)n(ater's)f(dy-)-150 1349 |
1512 |
< |
y(namical)19 b(prop)r(erties)g(3)h(and)f(4-p)r(oin)n(t)h(mo)r(dels.) |
1513 |
< |
1303 1319 y Fn(8)1360 1349 y Fu(This)g(attractiv)n(e)-150 |
1514 |
< |
1445 y(com)n(bination)33 b(of)i(sp)r(eed)f(and)g(accurate)f(depiction)h |
1507 |
> |
(while)g(main-)-150 1063 y(taining)37 b(the)g(structural)f(b)r(eha)n |
1508 |
> |
(vior)g(of)h(w)n(ater.)1364 1033 y Fn(5)1437 1063 y Fu(In)h(the)f |
1509 |
> |
(origi-)-150 1158 y(nal)31 b(molecular)f(dynamics)g(studies,)i(it)f(w)n |
1510 |
> |
(as)f(sho)n(wn)g(that)i(SSD)-150 1254 y(impro)n(v)n(es)g(on)h(the)g |
1511 |
> |
(prediction)g(of)h(man)n(y)e(of)i(w)n(ater's)e(dynami-)-150 |
1512 |
> |
1349 y(cal)e(prop)r(erties)g(o)n(v)n(er)f(TIP3P)g(and)i(SPC/E.)1282 |
1513 |
> |
1319 y Fn(8)1349 1349 y Fu(This)g(attractiv)n(e)-150 |
1514 |
> |
1445 y(com)n(bination)i(of)i(sp)r(eed)f(and)g(accurate)f(depiction)h |
1515 |
|
(of)h(solv)n(en)n(t)-150 1540 y(prop)r(erties)24 b(mak)n(es)h(SSD)h(a)e |
1516 |
|
(mo)r(del)i(of)f(in)n(terest)g(for)g(the)g(sim)n(ula-)-150 |
1517 |
|
1636 y(tion)k(of)g(large)e(scale)h(biological)f(systems,)i(suc)n(h)f |
1549 |
|
(estigators)-150 3545 y(of)f(the)g(SSD)h(w)n(ater)e(mo)r(del)h(ha)n(v)n |
1550 |
|
(e)e(put)j(forth)e(adjustmen)n(ts)i(to)-150 3641 y(the)30 |
1551 |
|
b(original)e(SSD)j(w)n(ater)d(mo)r(del)i(to)g(address)e(abnormal)h |
1552 |
< |
(den-)-150 3736 y(sit)n(y)i(b)r(eha)n(vior,)h(calling)f(the)h |
1553 |
< |
(corrected)e(mo)r(del)i(SSD1.)1628 3706 y Fn(10)1730 |
1554 |
< |
3736 y Fu(This)-150 3831 y(study)39 b(will)h(consider)e(this)i(new)f |
1555 |
< |
(mo)r(del's)g(b)r(eha)n(vior)f(as)h(w)n(ell,)-150 3927 |
1556 |
< |
y(and)26 b(hop)r(efully)g(impro)n(v)n(e)f(up)r(on)h(its)g(depiction)g |
1557 |
< |
(of)g(w)n(ater)f(under)-150 4022 y(conditions)i(without)h(the)g(Ew)n |
1558 |
< |
(ald)f(Sum.)552 4299 y Fo(I)r(I.)89 b(METHODS)-67 4512 |
1559 |
< |
y Fu(As)50 b(stated)h(previously)-7 b(,)55 b(in)50 b(this)h(study)f |
1560 |
< |
(the)h(long-range)-150 4608 y(dip)r(ole-dip)r(ole)37 |
1561 |
< |
b(in)n(teractions)f(w)n(ere)g(accoun)n(ted)h(for)f(using)h(the)-150 |
1562 |
< |
4703 y(reaction)h(\014eld)h(metho)r(d.)70 b(The)39 b(magnitude)g(of)f |
1563 |
< |
(the)i(reaction)-150 4799 y(\014eld)28 b(acting)f(on)g(dip)r(ole)h |
1564 |
< |
Fm(i)37 b Fu(is)27 b(giv)n(en)g(b)n(y)303 5024 y Ff(E)347 |
1565 |
< |
5036 y Fi(i)397 5024 y Fu(=)495 4968 y(2\()p Fj(")608 |
1566 |
< |
4980 y Fi(s)661 4968 y Ff(\000)18 b Fu(1\))p 495 5005 |
1567 |
< |
324 4 v 527 5081 a(2)p Fj(")608 5093 y Fi(s)661 5081 |
1568 |
< |
y Fu(+)g(1)856 4968 y(1)p 838 5005 78 4 v 838 5081 a |
1569 |
< |
Fj(r)877 5057 y Fn(3)875 5102 y Fi(c)945 4946 y Fg(X)939 |
1570 |
< |
5124 y Fi(j)s Ft(2R)1085 5024 y Fe(\026)1144 5045 y Fi(j)1179 |
1571 |
< |
5024 y Fj(f)9 b Fu(\()p Fj(r)1298 5036 y Fi(ij)1357 5024 |
1572 |
< |
y Fu(\))28 b Fj(;)346 b Fu(\(7\))-150 5297 y(where)32 |
1573 |
< |
b Ff(R)h Fu(is)f(the)h(ca)n(vit)n(y)e(de\014ned)h(b)n(y)h(the)f |
1574 |
< |
(cuto\013)h(radius)e(\()p Fj(r)1802 5309 y Fi(c)1837 |
1575 |
< |
5297 y Fu(\),)-150 5392 y Fj(")-111 5404 y Fi(s)-43 5392 |
1576 |
< |
y Fu(is)i(the)h(dielectric)f(constan)n(t)f(imp)r(osed)h(on)g(the)g |
1577 |
< |
(system)g(\(80)2042 -83 y(in)j(this)h(case\),)h Fe(\026)2619 |
1578 |
< |
-63 y Fi(j)2690 -83 y Fu(is)f(the)g(dip)r(ole)f(momen)n(t)g(v)n(ector)g |
1579 |
< |
(of)g(parti-)2042 24 y(cle)43 b Fm(j)p Fu(,)48 b(and)43 |
1580 |
< |
b Fj(f)9 b Fu(\()p Fj(r)2574 36 y Fi(ij)2632 24 y Fu(\))44 |
1581 |
< |
b(is)f(a)g(cubic)g(switc)n(hing)g(function.)3827 -6 y |
1582 |
< |
Fn(11)3941 24 y Fu(The)2042 120 y(reaction)c(\014eld)h(con)n(tribution) |
1583 |
< |
f(to)h(the)h(total)f(energy)f(b)n(y)g(par-)2042 215 y(ticle)f |
1584 |
< |
Fm(i)48 b Fu(is)38 b(giv)n(en)g(b)n(y)g Ff(\000)2828 |
1585 |
< |
183 y Fn(1)p 2827 197 34 4 v 2827 244 a(2)2870 215 y |
1586 |
< |
Fe(\026)2929 236 y Fi(i)2983 215 y Ff(\001)25 b(E)3075 |
1552 |
> |
(den-)-150 3736 y(sit)n(y)j(b)r(eha)n(vior)e(\(also)h(observ)n(ed)f |
1553 |
> |
(here\),)j(calling)f(the)g(corrected)-150 3831 y(mo)r(del)24 |
1554 |
> |
b(SSD1.)313 3801 y Fn(10)408 3831 y Fu(This)g(study)g(will)g(consider)f |
1555 |
> |
(this)h(new)g(mo)r(del's)-150 3927 y(b)r(eha)n(vior)30 |
1556 |
> |
b(as)g(w)n(ell,)h(and)g(hop)r(efully)h(impro)n(v)n(e)d(up)r(on)i(its)h |
1557 |
> |
(depic-)-150 4022 y(tion)c(of)f(w)n(ater)g(under)g(conditions)g |
1558 |
> |
(without)h(the)g(Ew)n(ald)f(Sum.)552 4299 y Fo(I)r(I.)89 |
1559 |
> |
b(METHODS)-67 4512 y Fu(As)50 b(stated)h(previously)-7 |
1560 |
> |
b(,)55 b(in)50 b(this)h(study)f(the)h(long-range)-150 |
1561 |
> |
4608 y(dip)r(ole-dip)r(ole)37 b(in)n(teractions)f(w)n(ere)g(accoun)n |
1562 |
> |
(ted)h(for)f(using)h(the)-150 4703 y(reaction)h(\014eld)h(metho)r(d.)70 |
1563 |
> |
b(The)39 b(magnitude)g(of)f(the)i(reaction)-150 4799 |
1564 |
> |
y(\014eld)28 b(acting)f(on)g(dip)r(ole)h Fm(i)37 b Fu(is)27 |
1565 |
> |
b(giv)n(en)g(b)n(y)303 5024 y Ff(E)347 5036 y Fi(i)397 |
1566 |
> |
5024 y Fu(=)495 4968 y(2\()p Fj(")608 4980 y Fi(s)661 |
1567 |
> |
4968 y Ff(\000)18 b Fu(1\))p 495 5005 324 4 v 527 5081 |
1568 |
> |
a(2)p Fj(")608 5093 y Fi(s)661 5081 y Fu(+)g(1)856 4968 |
1569 |
> |
y(1)p 838 5005 78 4 v 838 5081 a Fj(r)877 5057 y Fn(3)875 |
1570 |
> |
5102 y Fi(c)945 4946 y Fg(X)939 5124 y Fi(j)s Ft(2R)1085 |
1571 |
> |
5024 y Fe(\026)1144 5045 y Fi(j)1179 5024 y Fj(f)9 b |
1572 |
> |
Fu(\()p Fj(r)1298 5036 y Fi(ij)1357 5024 y Fu(\))28 b |
1573 |
> |
Fj(;)346 b Fu(\(7\))-150 5297 y(where)32 b Ff(R)h Fu(is)f(the)h(ca)n |
1574 |
> |
(vit)n(y)e(de\014ned)h(b)n(y)h(the)f(cuto\013)h(radius)e(\()p |
1575 |
> |
Fj(r)1802 5309 y Fi(c)1837 5297 y Fu(\),)-150 5392 y |
1576 |
> |
Fj(")-111 5404 y Fi(s)-43 5392 y Fu(is)i(the)h(dielectric)f(constan)n |
1577 |
> |
(t)f(imp)r(osed)h(on)g(the)g(system)g(\(80)2042 -83 y(in)j(this)h |
1578 |
> |
(case\),)h Fe(\026)2619 -63 y Fi(j)2690 -83 y Fu(is)f(the)g(dip)r(ole)f |
1579 |
> |
(momen)n(t)g(v)n(ector)g(of)g(parti-)2042 24 y(cle)43 |
1580 |
> |
b Fm(j)p Fu(,)48 b(and)43 b Fj(f)9 b Fu(\()p Fj(r)2574 |
1581 |
> |
36 y Fi(ij)2632 24 y Fu(\))44 b(is)f(a)g(cubic)g(switc)n(hing)g |
1582 |
> |
(function.)3827 -6 y Fn(11)3941 24 y Fu(The)2042 120 |
1583 |
> |
y(reaction)c(\014eld)h(con)n(tribution)f(to)h(the)h(total)f(energy)f(b) |
1584 |
> |
n(y)g(par-)2042 215 y(ticle)f Fm(i)48 b Fu(is)38 b(giv)n(en)g(b)n(y)g |
1585 |
> |
Ff(\000)2828 183 y Fn(1)p 2827 197 34 4 v 2827 244 a(2)2870 |
1586 |
> |
215 y Fe(\026)2929 236 y Fi(i)2983 215 y Ff(\001)25 b(E)3075 |
1587 |
|
227 y Fi(i)3141 215 y Fu(and)38 b(the)h(torque)f(on)g(dip)r(ole)2042 |
1588 |
|
320 y Fm(i)47 b Fu(b)n(y)38 b Fe(\026)2298 340 y Fi(i)2351 |
1589 |
|
320 y Ff(\002)25 b(E)2485 332 y Fi(i)2513 320 y Fu(.)2536 |
1609 |
|
y(isothermal)28 b(and)g(micro)r(canonical)f(ensem)n(bles.)40 |
1610 |
|
b(The)29 b(constan)n(t)2042 1657 y(pressure)c(sim)n(ulations)g(w)n(ere) |
1611 |
|
g(implemen)n(ted)i(using)f(an)f(in)n(tegral)2042 1752 |
1612 |
< |
y(thermostat)i(and)h(barostat)f(as)h(outlined)g(b)n(y)g(Ho)r(o)n(v)n |
1613 |
< |
(er.)3781 1722 y Fn(13)n(,14)3963 1752 y Fu(F)-7 b(or)2042 |
1614 |
< |
1848 y(the)34 b(constan)n(t)e(pressure)g(sim)n(ulations,)i(the)g |
1615 |
< |
Fm(Q)41 b Fu(parameter)32 b(for)2042 1943 y(the)e(w)n(as)f(set)h(to)g |
1616 |
< |
(5.0)f(am)n(u)g Ff(\001)2928 1928 y Fu(\027)2928 1943 |
1617 |
< |
y(A)2990 1913 y Fn(2)3028 1943 y Fu(,)h(and)g(the)g(relaxation)e(time)j |
1618 |
< |
(\()p Fj(\034)9 b Fu(\))2042 2038 y(w)n(as)26 b(set)i(at)f(100)g(ps.) |
1619 |
< |
2125 2134 y(In)n(tegration)e(of)h(the)g(equations)f(of)h(motion)g(w)n |
1620 |
< |
(as)f(carried)g(out)2042 2229 y(using)h(the)g(symplectic)h(splitting)g |
1621 |
< |
(metho)r(d)f(prop)r(osed)g(b)n(y)g(Dull-)2042 2325 y(w)n(eb)r(er)37 |
1622 |
< |
b Fm(et)i(al.)p Fu(.)2508 2295 y Fn(15)2618 2325 y Fu(The)f(reason)f |
1623 |
< |
(for)g(this)i(in)n(tegrator)d(selection)2042 2420 y(deals)g(with)h(p)r |
1612 |
> |
y(thermostat)k(and)h(barostat)f(as)g(outlined)h(b)n(y)g(Ho)r(o)n(v)n |
1613 |
> |
(er.)3792 1722 y Fn(13)o(,14)3976 1752 y Fu(All)2042 |
1614 |
> |
1848 y(particles)42 b(w)n(ere)g(treated)h(as)f(non-linear)g(rigid)h(b)r |
1615 |
> |
(o)r(dies.)83 b(Vi-)2042 1943 y(brational)27 b(constrain)n(ts)h(are)g |
1616 |
> |
(not)h(necessary)e(in)i(sim)n(ulations)f(of)2042 2038 |
1617 |
> |
y(SSD,)h(b)r(ecause)f(there)h(are)e(no)h(explicit)h(h)n(ydrogen)e |
1618 |
> |
(atoms,)h(and)2042 2134 y(th)n(us)j(no)f(molecular)g(vibrational)f(mo)r |
1619 |
> |
(des)h(need)h(to)g(b)r(e)g(consid-)2042 2229 y(ered.)2125 |
1620 |
> |
2325 y(In)n(tegration)25 b(of)h(the)g(equations)f(of)h(motion)g(w)n(as) |
1621 |
> |
f(carried)g(out)2042 2420 y(using)h(the)g(symplectic)h(splitting)g |
1622 |
> |
(metho)r(d)f(prop)r(osed)g(b)n(y)g(Dull-)2042 2516 y(w)n(eb)r(er)37 |
1623 |
> |
b Fm(et)i(al.)p Fu(.)2508 2486 y Fn(15)2618 2516 y Fu(The)f(reason)f |
1624 |
> |
(for)g(this)i(in)n(tegrator)d(selection)2042 2611 y(deals)g(with)h(p)r |
1625 |
|
(o)r(or)f(energy)f(conserv)-5 b(ation)36 b(of)g(rigid)g(b)r(o)r(dy)h |
1626 |
< |
(sys-)2042 2516 y(tems)24 b(using)h(quaternions.)34 b(While)25 |
1627 |
< |
b(quaternions)e(w)n(ork)h(w)n(ell)g(for)2042 2611 y(orien)n(tational)33 |
1626 |
> |
(sys-)2042 2707 y(tems)24 b(using)h(quaternions.)34 b(While)25 |
1627 |
> |
b(quaternions)e(w)n(ork)h(w)n(ell)g(for)2042 2802 y(orien)n(tational)33 |
1628 |
|
b(motion)h(in)h(alternate)e(ensem)n(bles,)j(the)f(micro-)2042 |
1629 |
< |
2707 y(canonical)j(ensem)n(ble)i(has)f(a)g(constan)n(t)g(energy)g |
1630 |
< |
(requiremen)n(t)2042 2802 y(that)27 b(is)h(actually)f(quite)g(sensitiv) |
1631 |
< |
n(e)g(to)g(errors)f(in)h(the)h(equations)2042 2898 y(of)e(motion.)37 |
1632 |
< |
b(The)27 b(original)e(implemen)n(tation)i(of)f(this)h(co)r(de)g(uti-) |
1633 |
< |
2042 2993 y(lized)19 b(quaternions)e(for)h(rotational)f(motion)i |
1634 |
< |
(propagation;)g(ho)n(w-)2042 3089 y(ev)n(er,)32 b(a)g(detailed)g(in)n |
1635 |
< |
(v)n(estigation)f(sho)n(w)n(ed)g(that)i(they)f(resulted)2042 |
1636 |
< |
3184 y(in)d(a)f(steady)g(drift)h(in)g(the)g(total)g(energy)-7 |
1637 |
< |
b(,)28 b(something)g(that)h(has)2042 3280 y(b)r(een)f(observ)n(ed)e(b)n |
1638 |
< |
(y)h(others.)2941 3250 y Fn(16)2125 3375 y Fu(The)d(k)n(ey)g |
1629 |
> |
2898 y(canonical)j(ensem)n(ble)i(has)f(a)g(constan)n(t)g(energy)g |
1630 |
> |
(requiremen)n(t)2042 2993 y(that)33 b(is)g(quite)g(sensitiv)n(e)g(to)f |
1631 |
> |
(errors)f(in)i(the)h(equations)e(of)h(mo-)2042 3089 y(tion.)57 |
1632 |
> |
b(The)34 b(original)f(implemen)n(tation)i(of)f(this)g(co)r(de)h |
1633 |
> |
(utilized)2042 3184 y(quaternions)27 b(for)g(rotational)f(motion)i |
1634 |
> |
(propagation;)e(ho)n(w)n(ev)n(er,)2042 3280 y(a)35 b(detailed)h(in)n(v) |
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< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19429 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19430 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19431 |
< |
% 00000000000000000000 |
19432 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19433 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19434 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19435 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19436 |
< |
% 00000000000000000000000000000000000000000000bb3300000000000000ff000011ff000000ff |
19437 |
< |
% 000066220055ee990000669900000000118800000022bb00000000005599110088ff000000000000 |
19438 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19439 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19440 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19441 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19442 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19443 |
< |
% 00000000000000000000 |
19444 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19445 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19446 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19447 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19448 |
< |
% 00000000000000000000000000000000000000000000ff0000000000000000ff000000ff000000ff |
19449 |
< |
% 00001100000055ff0000aa550011bbffcc3300000000ff0000000000cc11000022ff000000000000 |
19450 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19451 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19452 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19453 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19454 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19455 |
< |
% 00000000000000000000 |
19456 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19457 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19458 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19459 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19460 |
< |
% 00000000000000000000000000000000000000000000ff0000000000000000ff000000ff000000ff |
19461 |
< |
% 00000000000000ee0000ee0000bb110099dd00000000ff0000000000ff00000000ff000000000000 |
19462 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19463 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19464 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19465 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19466 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19467 |
< |
% 00000000000000000000 |
19468 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19469 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19470 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19471 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19472 |
< |
% 00000000000000000000000000000000000000000000ff0000000000000000ff110000ff110000ff |
19473 |
< |
% 00005533000033880055990000ee220000ee00000000ff0000000000ee77000000ff000000000000 |
19474 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19475 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19476 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19477 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19478 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19479 |
< |
% 00000000000000000000 |
19480 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19481 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19482 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19483 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19484 |
< |
% 00000000000000000000000000000000000000000000bb4400000000000000aaffcc66ffffaa77ff |
19485 |
< |
% 330088ddffffbb1100995500bbffcceeaa5500000011dd000000000099ee770011dd000000000000 |
19486 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19487 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19488 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19489 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19490 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19491 |
< |
% 00000000000000000000 |
19492 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19493 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19494 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19495 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19496 |
< |
% 00000000000000000000000000000000000000000000667700000000000000000000000000000055 |
19497 |
< |
% 110000000000000000dd0000001166110000000000559900000000001199ffffcc33000000000000 |
19498 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19499 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19500 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19501 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19502 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19503 |
< |
% 00000000000000000000 |
19504 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19505 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19506 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19507 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19508 |
< |
% 0000000000000000000000000000000000000000000000aa00000000000000000000000000000000 |
19509 |
< |
% 00000000000000005599000000000000000000000099220000000000000000000000000000000000 |
19510 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19511 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19512 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19513 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19514 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19515 |
< |
% 00000000000000000000 |
19516 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19517 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19518 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19519 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19520 |
< |
% 00000000000000000000000000000000000000000000003366003355556600000000000000000000 |
19521 |
< |
% 00000000000000009955000000000000000000006666000000000000000000000000000000000000 |
19522 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19523 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19524 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19525 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19526 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19527 |
< |
% 00000000000000000000 |
19528 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19529 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19530 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19531 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19532 |
< |
% 0000000000000000000000000000000000000000000000003333dd00000000000000000000000000 |
19533 |
< |
% 0000000000000000dd00000000000000000000224400000000000000000000000000000000000000 |
19534 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19535 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19536 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19537 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19538 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19539 |
< |
% 00000000000000000000 |
19540 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19541 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19542 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19543 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19544 |
< |
% 0000000000000000000000000000000000000000000000000000aa88330000000000000000000000 |
19545 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19546 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19547 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19548 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19549 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19550 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19551 |
< |
% 00000000000000000000 |
19552 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19553 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19554 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19555 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19556 |
< |
% 00000000000000000000000000000000000000000000000000002288000000000000000000000000 |
19557 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19558 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19559 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19560 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19561 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19562 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19563 |
< |
% 00000000000000000000 |
19564 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19565 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19566 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19567 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19568 |
< |
% 0000000000000000000000000000000000000000000000000000ee33003300000000000000000000 |
19569 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19570 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19571 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19572 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19573 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19574 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19575 |
< |
% 00000000000000000000 |
19576 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19577 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19578 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19579 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19580 |
< |
% 000000000000000000000000000000000000000000000000000066eecc1100000000000000000000 |
19581 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19582 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19583 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19584 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19585 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19586 |
< |
% 00000000000000000000000000000000000000000000000000000000000000000000000000000000 |
19587 |
< |
% 00000000000000000000 |
19588 |
< |
%%EndImage |
19589 |
< |
%%EndPreview |
19590 |
< |
save countdictstack mark newpath /showpage {} def /setpagedevice {pop} def |
19591 |
< |
%%EndProlog |
19592 |
< |
%%Page: 1 1 |
19593 |
< |
%%BeginDocument: 1hdense.ps |
19594 |
< |
80 dict begin |
19595 |
< |
/languagelevel where |
19596 |
< |
{pop /gs_languagelevel languagelevel def} |
19597 |
< |
{/gs_languagelevel 1 def} ifelse |
19598 |
< |
gs_languagelevel 1 gt { |
19599 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19600 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19601 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19602 |
< |
{<0000000000000000000000000000000000000000000000000000000000000000>} image end } |
19603 |
< |
>> matrix makepattern /Pat0 exch def |
19604 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19605 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19606 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19607 |
< |
{<1111000044440000111100004444000011110000444400001111000044440000>} image end } |
19608 |
< |
>> matrix makepattern /Pat1 exch def |
19609 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19610 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19611 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19612 |
< |
{<1111444411114444111144441111444411114444111144441111444411114444>} image end } |
19613 |
< |
>> matrix makepattern /Pat2 exch def |
19614 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19615 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19616 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19617 |
< |
{<aaaa5555aaaa5555aaaa5555aaaa5555aaaa5555aaaa5555aaaa5555aaaa5555>} image end } |
19618 |
< |
>> matrix makepattern /Pat3 exch def |
19619 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19620 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19621 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19622 |
< |
{<eeeebbbbeeeebbbbeeeebbbbeeeebbbbeeeebbbbeeeebbbbeeeebbbbeeeebbbb>} image end } |
19623 |
< |
>> matrix makepattern /Pat4 exch def |
19624 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19625 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19626 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19627 |
< |
{<eeeeffffbbbbffffeeeeffffbbbbffffeeeeffffbbbbffffeeeeffffbbbbffff>} image end } |
19628 |
< |
>> matrix makepattern /Pat5 exch def |
19629 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19630 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19631 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19632 |
< |
{<f77dffffbeeffffff77dffffbeeffffff77dffffbeeffffff77dffffbeefffff>} image end } |
19633 |
< |
>> matrix makepattern /Pat6 exch def |
19634 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19635 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19636 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19637 |
< |
{<ffffffffffffffffffffffffffffffffffffffffffffffffffffffffffffffff>} image end } |
19638 |
< |
>> matrix makepattern /Pat7 exch def |
19639 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19640 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19641 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19642 |
< |
{<e1e1f0f078783c3c1e1e0f0f8787c3c3e1e1f0f078783c3c1e1e0f0f8787c3c3>} image end } |
19643 |
< |
>> matrix makepattern /Pat8 exch def |
19644 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19645 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19646 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19647 |
< |
{<87870f0f1e1e3c3c7878f0f0e1e1c3c387870f0f1e1e3c3c7878f0f0e1e1c3c3>} image end } |
19648 |
< |
>> matrix makepattern /Pat9 exch def |
19649 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19650 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19651 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19652 |
< |
{<cccccccccccccccccccccccccccccccccccccccccccccccccccccccccccccccc>} image end } |
19653 |
< |
>> matrix makepattern /Pat10 exch def |
19654 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19655 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19656 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19657 |
< |
{<00000000ffffffff00000000ffffffff00000000ffffffff00000000ffffffff>} image end } |
19658 |
< |
>> matrix makepattern /Pat11 exch def |
19659 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19660 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19661 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19662 |
< |
{<7e7ebdbddbdbe7e7e7e7dbdbbdbd7e7e7e7ebdbddbdbe7e7e7e7dbdbbdbd7e7e>} image end } |
19663 |
< |
>> matrix makepattern /Pat12 exch def |
19664 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19665 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19666 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19667 |
< |
{<fd7e7ebfbfdfdfefeff7f7fbfbfdfd7e7ebfbfdfdfefeff7f7fbfbfdfd7e7ebf>} image end } |
19668 |
< |
>> matrix makepattern /Pat13 exch def |
19669 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19670 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19671 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19672 |
< |
{<7ebffd7efbfdf7fbeff7dfefbfdf7ebffd7efbfdf7fbeff7dfefbfdf7ebffd7e>} image end } |
19673 |
< |
>> matrix makepattern /Pat14 exch def |
19674 |
< |
<</PaintType 1 /PatternType 1 /TilingType 1 |
19675 |
< |
/BBox [0 0 12 12] /XStep 12 /YStep 12 /PaintProc{ begin |
19676 |
< |
12 12 scale 16 16 1 [16 0 0 16 0 0] |
19677 |
< |
{<fffffbdff3dfebdfdbdfbbdf7bdffbdefbddfbdbfbd7fbcffbdfffffffffffff>} image end } |
19678 |
< |
>> matrix makepattern /Pat15 exch def |
19679 |
< |
}{ |
19680 |
< |
/Pat0 { 0.000000 setgray } def |
19681 |
< |
/Pat1 { 0.062500 setgray } def |
19682 |
< |
/Pat2 { 0.125000 setgray } def |
19683 |
< |
/Pat3 { 0.187500 setgray } def |
19684 |
< |
/Pat4 { 0.250000 setgray } def |
19685 |
< |
/Pat5 { 0.312500 setgray } def |
19686 |
< |
/Pat6 { 0.375000 setgray } def |
19687 |
< |
/Pat7 { 0.437500 setgray } def |
19688 |
< |
/Pat8 { 0.500000 setgray } def |
19689 |
< |
/Pat9 { 0.562500 setgray } def |
19690 |
< |
/Pat10 { 0.625000 setgray } def |
19691 |
< |
/Pat11 { 0.687500 setgray } def |
19692 |
< |
/Pat12 { 0.750000 setgray } def |
19693 |
< |
/Pat13 { 0.812500 setgray } def |
19694 |
< |
/Pat14 { 0.875000 setgray } def |
19695 |
< |
/Pat15 { 0.937500 setgray } def |
19696 |
< |
/setpattern { } def |
19697 |
< |
} ifelse |
19698 |
< |
/m {moveto} bind def |
19699 |
< |
/l {lineto} bind def |
19700 |
< |
/s {stroke} bind def |
19701 |
< |
% Symbol fill |
19702 |
< |
/f { gsave fill grestore stroke } bind def |
19703 |
< |
% Opaque symbol |
19704 |
< |
/o { gsave 1.000000 1.000000 1.000000 setrgbcolor |
19705 |
< |
fill grestore stroke } bind def |
19706 |
< |
% Circle symbol |
19707 |
< |
/a { 3 -1 roll 0 360 arc } bind def |
19708 |
< |
/da { a s } bind def |
19709 |
< |
/fa { a f } bind def |
19710 |
< |
/oa { a o } bind def |
19711 |
< |
% Square symbol |
19712 |
< |
/sq { moveto dup dup rmoveto 2 mul |
19713 |
< |
dup neg 0 rlineto dup neg 0 exch rlineto |
19714 |
< |
0 rlineto closepath } bind def |
19715 |
< |
/dsq { sq s } bind def |
19716 |
< |
/fsq { sq f } bind def |
19717 |
< |
/osq { sq o } bind def |
19718 |
< |
% Triangle symbols |
19719 |
< |
/t1 { moveto dup 0 exch rmoveto |
19720 |
< |
dup neg dup 2 mul rlineto 2 mul 0 rlineto |
19721 |
< |
closepath } bind def |
19722 |
< |
/dt1 { t1 s } bind def |
19723 |
< |
/ft1 { t1 f } bind def |
19724 |
< |
/ot1 { t1 o } bind def |
19725 |
< |
/t2 { moveto dup neg 0 rmoveto |
19726 |
< |
dup dup 2 mul exch neg rlineto |
19727 |
< |
2 mul 0 exch rlineto closepath } bind def |
19728 |
< |
/dt2 { t2 s } bind def |
19729 |
< |
/ft2 { t2 f } bind def |
19730 |
< |
/ot2 { t2 o } bind def |
19731 |
< |
/t3 { moveto dup neg 0 exch rmoveto |
19732 |
< |
dup dup 2 mul rlineto neg 2 mul 0 rlineto |
19733 |
< |
closepath } bind def |
19734 |
< |
/dt3 { t3 s } bind def |
19735 |
< |
/ft3 { t3 f } bind def |
19736 |
< |
/ot3 { t3 o } bind def |
19737 |
< |
/t4 { moveto dup 0 rmoveto |
19738 |
< |
dup dup -2 mul exch rlineto |
19739 |
< |
-2 mul 0 exch rlineto closepath } bind def |
19740 |
< |
/dt4 { t4 s } bind def |
19741 |
< |
/ft4 { t4 f } bind def |
19742 |
< |
/ot4 { t4 o } bind def |
19743 |
< |
% Diamond symbol |
19744 |
< |
/di { moveto dup 0 exch rmoveto |
19745 |
< |
dup neg dup rlineto dup dup neg rlineto |
19746 |
< |
dup dup rlineto closepath } bind def |
19747 |
< |
/ddi { di s } bind def |
19748 |
< |
/fdi { di f } bind def |
19749 |
< |
/odi { di o } bind def |
19750 |
< |
% Plus symbol |
19751 |
< |
/pl { dup 0 rmoveto dup -2 mul 0 rlineto |
19752 |
< |
dup dup rmoveto -2 mul 0 exch rlineto |
19753 |
< |
} bind def |
19754 |
< |
/dpl { m pl s } bind def |
19755 |
< |
% x symbol |
19756 |
< |
/x { dup dup rmoveto dup -2 mul dup rlineto |
19757 |
< |
2 mul dup 0 rmoveto dup neg exch rlineto |
19758 |
< |
} bind def |
19759 |
< |
/dx { m x s } bind def |
19760 |
< |
% Splat symbol |
19761 |
< |
/dsp { m dup pl dup 0 exch rmoveto 0.707 mul x s |
19762 |
< |
} bind def |
19763 |
< |
/RJ { |
19764 |
< |
stringwidth neg exch neg exch |
19765 |
< |
rmoveto |
19766 |
< |
} bind def |
19767 |
< |
/CS { |
19768 |
< |
stringwidth |
19769 |
< |
2 div neg exch 2 div neg exch |
19770 |
< |
rmoveto |
19771 |
< |
} bind def |
19772 |
< |
0.24 0.24 scale |
19773 |
< |
1 setlinecap |
19774 |
< |
|
19775 |
< |
mark |
19776 |
< |
/ISOLatin1Encoding |
19777 |
< |
8#000 1 8#054 {StandardEncoding exch get} for |
19778 |
< |
/minus |
19779 |
< |
8#056 1 8#217 {StandardEncoding exch get} for |
19780 |
< |
/dotlessi |
19781 |
< |
8#301 1 8#317 {StandardEncoding exch get} for |
19782 |
< |
/space /exclamdown /cent /sterling /currency /yen /brokenbar /section |
19783 |
< |
/dieresis /copyright /ordfeminine /guillemotleft /logicalnot /hyphen |
19784 |
< |
/registered /macron /degree /plusminus /twosuperior /threesuperior /acute |
19785 |
< |
/mu /paragraph /periodcentered /cedilla /onesuperior /ordmasculine |
19786 |
< |
/guillemotright /onequarter /onehalf /threequarters /questiondown /Agrave |
19787 |
< |
/Aacute /Acircumflex /Atilde /Adieresis /Aring /AE /Ccedilla /Egrave /Eacute |
19788 |
< |
/Ecircumflex /Edieresis /Igrave /Iacute /Icircumflex /Idieresis /Eth /Ntilde |
19789 |
< |
/Ograve /Oacute /Ocircumflex /Otilde /Odieresis /multiply /Oslash /Ugrave |
19790 |
< |
/Uacute /Ucircumflex /Udieresis /Yacute /Thorn /germandbls /agrave /aacute |
19791 |
< |
/acircumflex /atilde /adieresis /aring /ae /ccedilla /egrave /eacute |
19792 |
< |
/ecircumflex /edieresis /igrave /iacute /icircumflex /idieresis /eth /ntilde |
19793 |
< |
/ograve /oacute /ocircumflex /otilde /odieresis /divide /oslash /ugrave |
19794 |
< |
/uacute /ucircumflex /udieresis /yacute /thorn /ydieresis |
19795 |
< |
/ISOLatin1Encoding where not {256 array astore def} if |
19796 |
< |
cleartomark |
19797 |
< |
|
19798 |
< |
/makeISOEncoded |
19799 |
< |
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19812 |
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19815 |
< |
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19816 |
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19818 |
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19819 |
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19821 |
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19823 |
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19824 |
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19826 |
< |
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< |
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19828 |
< |
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19844 |
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19845 |
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19847 |
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19848 |
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19849 |
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19852 |
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19854 |
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19856 |
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19857 |
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19858 |
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19860 |
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19861 |
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19862 |
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19863 |
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19864 |
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19865 |
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19866 |
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19867 |
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19868 |
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19869 |
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19870 |
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19871 |
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19876 |
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19878 |
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19879 |
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19880 |
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19881 |
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19882 |
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19883 |
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19885 |
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19886 |
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19887 |
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19888 |
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19889 |
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19890 |
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19891 |
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19892 |
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19894 |
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19895 |
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19899 |
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19900 |
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19910 |
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19912 |
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19926 |
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19930 |
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19931 |
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19935 |
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< |
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19944 |
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< |
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19951 |
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< |
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20050 |
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20051 |
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20052 |
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20054 |
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20055 |
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20056 |
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@endspecial 3590 -166 a |
12411 |
> |
@endspecial 1302 -166 a |
12412 |
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currentpoint grestore moveto |
12413 |
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3590 -166 a 2042 1513 a Fr(FIG.)28 |
12414 |
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b(2:)38 b(Av)n(erage)28 b(densit)n(y)e(of)j(SSD)d(w)n(ater)i(at)g |
12415 |
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Fq(I)2890 1609 y Fp(h)2955 1600 y Fr(lattice.)2042 1880 |
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y Fu(\014xed)d(p)r(ositions)f(with)i(angular)d(momen)n(ta)i(randomized) |
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f(at)h(400)2042 1975 y(K)40 b(for)g(v)-5 b(arying)39 |
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2071 y(then)f(scaled)g(do)n(wn)g(in)g(stages)f(to)h(slo)n(wly)f(co)r |
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1302 -166 a -150 1418 a Fr(FIG.)26 |
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> |
b(1:)34 b(Energy)26 b(conserv)l(ation)g(using)f(quaternion)h(based)f |
12415 |
> |
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12416 |
> |
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12417 |
> |
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12418 |
> |
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12419 |
> |
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12420 |
> |
(step)g(in)n(tegra-)-150 1767 y(tor,)h(and)e(the)h(solid)h(line)f |
12421 |
> |
(comes)g(from)g(the)f(quaternion)h(in)n(tegrator.)-150 |
12422 |
> |
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12423 |
> |
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12424 |
> |
-6 b(.)-150 2221 y Fu(arithmetic)28 b(quaternion)f(propagation.)35 |
12425 |
> |
b(With)29 b(the)g(same)e(time)-150 2317 y(step,)22 b(a)d(1000)f(SSD)i |
12426 |
> |
(particle)f(sim)n(ulation)h(sho)n(ws)e(an)i(a)n(v)n(erage)d(7\045)-150 |
12427 |
> |
2412 y(increase)32 b(in)i(computation)f(time)h(using)f(the)h |
12428 |
> |
(symplectic)f(step)-150 2508 y(metho)r(d)e(in)h(place)e(of)h |
12429 |
> |
(quaternions.)45 b(This)31 b(cost)f(is)h(more)f(than)-150 |
12430 |
> |
2603 y(justi\014ed)f(when)g(comparing)e(the)i(energy)f(conserv)-5 |
12431 |
> |
b(ation)27 b(of)h(the)-150 2699 y(t)n(w)n(o)f(metho)r(ds)h(as)f |
12432 |
> |
(illustrated)g(in)h(\014gure)f(1.)-67 2794 y(In)33 b(\014gure)f(1,)i |
12433 |
> |
(the)f(resulting)f(energy)g(drift)h(at)f(v)-5 b(arious)32 |
12434 |
> |
b(time)-150 2890 y(steps)h(for)f(b)r(oth)h(the)g(symplectic)g(step)f |
12435 |
> |
(and)h(quaternion)f(in)n(te-)-150 2985 y(gration)25 b(sc)n(hemes)h(is)g |
12436 |
> |
(compared.)36 b(All)27 b(of)f(the)h(1000)e(SSD)i(parti-)-150 |
12437 |
> |
3081 y(cle)g(sim)n(ulations)g(started)g(with)h(the)g(same)f |
12438 |
> |
(con\014guration,)f(and)-150 3176 y(the)40 b(only)f(di\013erence)h(w)n |
12439 |
> |
(as)f(the)h(metho)r(d)g(for)f(handling)h(rota-)-150 3272 |
12440 |
> |
y(tional)i(motion.)79 b(A)n(t)42 b(time)h(steps)f(of)f(0.1)g(and)h(0.5) |
12441 |
> |
f(fs,)46 b(b)r(oth)-150 3367 y(metho)r(ds)37 b(for)g(propagating)e |
12442 |
> |
(particle)h(rotation)g(conserv)n(e)g(en-)-150 3463 y(ergy)31 |
12443 |
> |
b(fairly)i(w)n(ell,)g(with)g(the)g(quaternion)f(metho)r(d)h(sho)n(wing) |
12444 |
> |
f(a)-150 3558 y(sligh)n(t)d(energy)g(drift)h(o)n(v)n(er)d(time)j(in)g |
12445 |
> |
(the)g(0.5)f(fs)h(time)g(step)g(sim-)-150 3653 y(ulation.)47 |
12446 |
> |
b(A)n(t)31 b(time)h(steps)f(of)g(1)f(and)h(2)g(fs,)h(the)f(energy)f |
12447 |
> |
(conser-)-150 3749 y(v)-5 b(ation)25 b(b)r(ene\014ts)h(of)g(the)g |
12448 |
> |
(symplectic)f(step)h(metho)r(d)g(are)f(clearly)-150 3844 |
12449 |
> |
y(demonstrated.)36 b(Th)n(us,)27 b(while)g(main)n(taining)g(the)g(same) |
12450 |
> |
f(degree)-150 3940 y(of)h(energy)f(conserv)-5 b(ation,)26 |
12451 |
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b(one)h(can)g(tak)n(e)f(considerably)g(longer)-150 4035 |
12452 |
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y(time)34 b(steps,)g(leading)f(to)g(an)g(o)n(v)n(erall)e(reduction)i |
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(in)g(computa-)-150 4131 y(tion)28 b(time.)-67 4226 y(Energy)23 |
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12455 |
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-150 4322 y(noticeable)36 b(for)h(time)g(steps)g(up)g(to)g(three)g(fem) |
12456 |
> |
n(toseconds.)64 b(A)-150 4417 y(sligh)n(t)40 b(energy)f(drift)i(on)f |
12457 |
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(the)h(order)e(of)h(0.012)f(k)n(cal/mol)f(p)r(er)-150 |
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4513 y(nanosecond)21 b(w)n(as)h(observ)n(ed)g(at)g(a)h(time)g(step)g |
12459 |
> |
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12460 |
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(ected,)i(this)e(drift)h(increases)e(dramatically)-150 |
12461 |
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4704 y(with)24 b(increasing)e(time)i(step.)35 b(T)-7 |
12462 |
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b(o)23 b(insure)g(accuracy)f(in)h(the)h(con-)-150 4799 |
12463 |
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y(stan)n(t)j(energy)f(sim)n(ulations,)h(time)h(steps)f(w)n(ere)f(set)i |
12464 |
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(at)f(2)g(fs)h(and)-150 4895 y(k)n(ept)38 b(at)g(this)g(v)-5 |
12465 |
> |
b(alue)38 b(for)f(constan)n(t)g(pressure)g(sim)n(ulations)g(as)-150 |
12466 |
> |
4990 y(w)n(ell.)-67 5086 y(Ice)g(crystals)e(in)i(b)r(oth)g(the)h |
12467 |
> |
Fj(I)886 5098 y Fi(h)966 5086 y Fu(and)f Fj(I)1173 5098 |
12468 |
> |
y Fi(c)1244 5086 y Fu(lattices)f(w)n(ere)g(gen-)-150 |
12469 |
> |
5181 y(erated)k(as)g(starting)g(p)r(oin)n(ts)g(for)g(all)g(the)h(sim)n |
12470 |
> |
(ulations.)75 b(The)-150 5277 y Fj(I)-114 5289 y Fi(h)-38 |
12471 |
> |
5277 y Fu(crystals)31 b(w)n(ere)h(formed)g(b)n(y)g(\014rst)g(arranging) |
12472 |
> |
e(the)j(cen)n(ter)e(of)-150 5372 y(masses)21 b(of)i(the)g(SSD)g |
12473 |
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(particles)f(in)n(to)g(a)g(\\hexagonal")e(ice)i(lattice)2042 |
12474 |
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-83 y(of)30 b(1024)f(particles.)45 b(Because)30 b(of)g(the)h(crystal)f |
12475 |
> |
(structure)g(of)h Fj(I)4041 -71 y Fi(h)2042 12 y Fu(ice,)23 |
12476 |
> |
b(the)f(sim)n(ulation)f(b)r(o)n(x)g(assumed)g(a)g(rectangular)e(shap)r |
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(e)j(with)2042 108 y(a)43 b(edge)g(length)g(ratio)g(of)g(appro)n |
12478 |
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(ximately)f(1.00)p Ff(\002)p Fu(1.06)p Ff(\002)p Fu(1.23.)2042 |
12479 |
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203 y(The)c(particles)g(w)n(ere)g(then)h(allo)n(w)n(ed)e(to)h(orien)n |
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(t)g(freely)g(ab)r(out)2042 299 y(\014xed)23 b(p)r(ositions)f(with)i |
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(angular)d(momen)n(ta)i(randomized)f(at)h(400)2042 394 |
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12490 |
> |
872 y(and)26 b(the)i(ice)e(crystals)g(w)n(ere)g(allo)n(w)n(ed)f(to)i |
12491 |
> |
(equilibrate)f(for)g(50)g(ps)2042 967 y(at)32 b(25)g(K)h(and)g(a)f |
12492 |
> |
(constan)n(t)g(pressure)g(of)g(1)h(atm.)52 b(This)33 |
12493 |
> |
b(pro)r(ce-)2042 1063 y(dure)i(resulted)g(in)h(structurally)f(stable)g |
12494 |
> |
Fj(I)3409 1075 y Fi(h)3488 1063 y Fu(ice)h(crystals)e(that)2042 |
12495 |
> |
1158 y(ob)r(ey)26 b(the)g(Bernal-F)-7 b(o)n(wler)24 b(rules)3084 |
12496 |
> |
1128 y Fn(17,18)3239 1158 y Fu(.)36 b(This)26 b(metho)r(d)h(w)n(as)e |
12497 |
> |
(also)2042 1254 y(utilized)j(in)h(the)f(making)f(of)h(diamond)g |
12498 |
> |
(lattice)g Fj(I)3598 1266 y Fi(c)3661 1254 y Fu(ice)f(crystals,)2042 |
12499 |
> |
1349 y(with)22 b(eac)n(h)f(cubic)h(sim)n(ulation)f(b)r(o)n(x)g |
12500 |
> |
(consisting)g(of)g(either)h(512)e(or)2042 1445 y(1000)30 |
12501 |
> |
b(particles.)51 b(Only)32 b(isotropic)f(v)n(olume)h(\015uctuations)g(w) |
12502 |
> |
n(ere)2042 1540 y(p)r(erformed)e(under)h(constan)n(t)f(pressure,)h(so)f |
12503 |
> |
(the)i(ratio)e(of)h(edge)2042 1636 y(lengths)c(remained)g(constan)n(t)g |
12504 |
> |
(throughout)g(the)h(sim)n(ulations.)2349 1912 y Fo(I)r(I)r(I.)90 |
12505 |
> |
b(RESUL)-7 b(TS)29 b(AND)g(DISCUSSION)2125 2125 y Fu(Melting)c(studies) |
12506 |
> |
g(w)n(ere)g(p)r(erformed)f(on)h(the)h(randomized)e(ice)2042 |
12507 |
> |
2221 y(crystals)18 b(using)i(constan)n(t)f(pressure)f(and)i(temp)r |
12508 |
> |
(erature)g(dynam-)2042 2316 y(ics.)84 b(This)44 b(in)n(v)n(olv)n(ed)e |
12509 |
> |
(an)h(initial)h(randomization)e(of)h(v)n(elo)r(ci-)2042 |
12510 |
> |
2412 y(ties)31 b(ab)r(out)h(the)f(starting)g(temp)r(erature)g(of)g(25)g |
12511 |
> |
(K)g(for)f(v)-5 b(arying)2042 2507 y(amoun)n(ts)31 b(of)i(time.)51 |
12512 |
> |
b(The)33 b(systems)e(w)n(ere)h(all)g(equilibrated)g(for)2042 |
12513 |
> |
2603 y(100)25 b(ps)h(prior)f(to)i(a)f(200)f(ps)h(data)g(collection)g |
12514 |
> |
(run)g(at)g(eac)n(h)g(tem-)2042 2698 y(p)r(erature)g(setting,)h |
12515 |
> |
(ranging)f(from)h(25)f(to)h(400)f(K,)h(with)g(a)g(max-)2042 |
12516 |
> |
2794 y(im)n(um)33 b(degree)f(incremen)n(t)h(of)g(25)f(K.)h(F)-7 |
12517 |
> |
b(or)32 b(regions)g(of)h(in)n(terest)2042 2889 y(along)i(this)i(step)n |
12518 |
> |
(wise)f(progression,)g(the)h(temp)r(erature)f(incre-)2042 |
12519 |
> |
2985 y(men)n(t)28 b(w)n(as)g(decreased)f(from)h(25)f(K)h(to)h(10)e(and) |
12520 |
> |
h(then)h(5)f(K.)g(The)2042 3080 y(ab)r(o)n(v)n(e)e(equilibration)i(and) |
12521 |
|
f(pro)r(duction)h(times)g(w)n(ere)f(su\016cien)n(t)2042 |
12522 |
< |
4757 y(in)g(that)g(the)g(system)f(v)n(olume)g(\015uctuations)h(damp)r |
12523 |
< |
(ened)g(out)g(in)2042 4852 y(all)34 b(but)g(the)h(v)n(ery)e(cold)g(sim) |
12524 |
< |
n(ulations)g(\(b)r(elo)n(w)h(225)f(K\).)h(In)g(or-)2042 |
12525 |
< |
4948 y(der)23 b(to)h(further)g(impro)n(v)n(e)e(statistics,)j(\014v)n(e) |
12526 |
< |
e(separate)g(sim)n(ulation)2042 5043 y(progressions)37 |
12527 |
< |
b(w)n(ere)i(p)r(erformed,)k(and)d(the)g(a)n(v)n(eraged)e(results)2042 |
12528 |
< |
5138 y(from)27 b(the)h Fj(I)2417 5150 y Fi(h)2488 5138 |
12529 |
< |
y Fu(melting)g(sim)n(ulations)f(are)f(sho)n(wn)h(in)h(\014gure)f(2.)p |
12530 |
< |
eop |
12522 |
> |
3175 y(in)g(that)g(the)g(system)f(v)n(olume)g(\015uctuations)h(damp)r |
12523 |
> |
(ened)g(out)g(in)2042 3271 y(all)e(but)h(the)f(v)n(ery)f(cold)h(sim)n |
12524 |
> |
(ulations)g(\(b)r(elo)n(w)g(225)f(K\).)h(In)h(order)2042 |
12525 |
> |
3366 y(to)38 b(further)g(impro)n(v)n(e)f(statistics,)j(an)e(ensem)n |
12526 |
> |
(ble)g(a)n(v)n(erage)d(w)n(as)2042 3462 y(accum)n(ulated)30 |
12527 |
> |
b(from)h(\014v)n(e)f(separate)g(sim)n(ulation)g(progressions,)2042 |
12528 |
> |
3557 y(eac)n(h)d(starting)f(from)i(a)f(di\013eren)n(t)g(ice)h(crystal.) |
12529 |
> |
2638 3834 y Fo(A.)88 b(Densit)n(y)29 b(Beha)n(vior)2125 |
12530 |
> |
4047 y Fu(In)e(the)h(initial)g(a)n(v)n(erage)d(densit)n(y)i(v)n(ersus)f |
12531 |
> |
(temp)r(erature)h(plot,)2042 4143 y(the)34 b(densit)n(y)g(maxim)n(um)g |
12532 |
> |
(clearly)f(app)r(ears)g(b)r(et)n(w)n(een)i(255)d(and)2042 |
12533 |
> |
4238 y(265)i(K.)h(The)h(calculated)f(densities)h(within)g(this)g(range) |
12534 |
> |
e(w)n(ere)2042 4334 y(nearly)f(indistinguishable,)i(as)e(can)g(b)r(e)h |
12535 |
> |
(seen)g(in)g(the)g(zo)r(om)f(of)2042 4429 y(this)g(region)f(of)h(in)n |
12536 |
> |
(terest,)h(sho)n(wn)e(in)h(\014gure)g Fh(??)p Fu(.)53 |
12537 |
> |
b(The)33 b(greater)2042 4525 y(certain)n(t)n(y)24 b(of)h(the)h(a)n(v)n |
12538 |
> |
(erage)c(v)-5 b(alue)26 b(at)f(260)f(K)h(mak)n(es)f(a)h(go)r(o)r(d)f |
12539 |
> |
(ar-)2042 4620 y(gumen)n(t)k(for)g(the)h(actual)f(densit)n(y)g(maxim)n |
12540 |
> |
(um)g(residing)g(at)g(this)2042 4715 y(midp)r(oin)n(t)j(v)-5 |
12541 |
> |
b(alue.)46 b(Figure)30 b Fh(??)i Fu(w)n(as)d(constructed)i(using)f(ice) |
12542 |
> |
h Fj(I)4041 4727 y Fi(h)2042 4811 y Fu(crystals)23 b(for)i(the)g |
12543 |
> |
(initial)g(con\014guration;)f(and)h(though)g(not)f(pic-)2042 |
12544 |
> |
4906 y(tured,)h(the)h(sim)n(ulations)e(starting)g(from)g(ice)h |
12545 |
> |
Fj(I)3517 4918 y Fi(c)3576 4906 y Fu(crystal)f(con\014g-)2042 |
12546 |
> |
5002 y(urations)h(sho)n(w)n(ed)h(similar)g(results,)g(with)h(a)f |
12547 |
> |
(liquid-phase)g(den-)2042 5097 y(sit)n(y)g(maxim)n(um)g(in)h(this)g |
12548 |
> |
(same)f(region)f(\(b)r(et)n(w)n(een)i(255)e(and)i(260)2042 |
12549 |
> |
5193 y(K\).)f(In)h(addition,)g(the)f Fj(I)2818 5205 y |
12550 |
> |
Fi(c)2879 5193 y Fu(crystals)g(are)f(more)h(fragile)f(than)i(the)2042 |
12551 |
> |
5288 y Fj(I)2078 5300 y Fi(h)2154 5288 y Fu(crystals,)34 |
12552 |
> |
b(leading)e(them)i(to)f(deform)f(in)n(to)h(a)g(dense)g(glassy)2042 |
12553 |
> |
5384 y(state)d(at)g(lo)n(w)n(er)f(temp)r(eratures.)45 |
12554 |
> |
b(This)30 b(resulted)h(in)f(an)g(o)n(v)n(erall)p eop |
12555 |
|
%%Page: 4 4 |
12556 |
|
4 3 bop 4043 -299 a Fu(4)-150 -166 y |
12557 |
|
gsave currentpoint currentpoint translate -90 neg rotate neg exch |
21676 |
|
@endspecial 1385 -166 a |
21677 |
|
currentpoint grestore moveto |
21678 |
|
1385 -166 a -150 1525 a Fr(FIG.)81 |
21679 |
< |
b(3:)144 b(Densit)n(y)80 b(v)n(ersus)g(temp)r(erature)g(for)h(TIP4P) |
21679 |
> |
b(2:)144 b(Densit)n(y)80 b(v)n(ersus)g(temp)r(erature)g(for)h(TIP4P) |
21680 |
|
1805 1493 y Fc(19)1871 1525 y Fr(,)-150 1612 y(TIP3P)75 |
21681 |
|
1580 y Fc(19)141 1612 y Fr(,)33 b(SPC/E)435 1580 y Fc(20)501 |
21682 |
|
1612 y Fr(,)g(SSD)d(without)i(Reaction)f(Field,)j(SSD,)d(and)-150 |
21683 |
< |
1699 y(Exp)r(erimen)n(t)243 1667 y Fc(21)307 1699 y Fr(.)446 |
21684 |
< |
1979 y Fo(A.)88 b(Densit)n(y)29 b(Beha)n(vior)-67 2193 |
21685 |
< |
y Fu(In)f(the)g(initial)f(a)n(v)n(erage)e(densit)n(y)i(v)n(ersus)f |
21686 |
< |
(temp)r(erature)h(plot,)-150 2288 y(the)35 b(densit)n(y)f(maxim)n(um)g |
21687 |
< |
(clearly)f(app)r(ears)g(b)r(et)n(w)n(een)h(255)f(and)-150 |
21688 |
< |
2384 y(265)h(K.)i(The)f(calculated)g(densities)h(within)g(this)g(range) |
21689 |
< |
e(w)n(ere)-150 2479 y(nearly)f(indistinguishable,)i(as)e(can)g(b)r(e)i |
21690 |
< |
(seen)e(in)h(the)g(zo)r(om)f(of)-150 2575 y(this)38 b(region)e(of)h(in) |
21691 |
< |
n(terest,)i(sho)n(wn)e(in)h(\014gure)e(2.)66 b(The)37 |
21692 |
< |
b(greater)-150 2670 y(certain)n(t)n(y)24 b(of)h(the)h(a)n(v)n(erage)d |
21693 |
< |
(v)-5 b(alue)25 b(at)g(260)f(K)h(mak)n(es)f(a)h(go)r(o)r(d)g(ar-)-150 |
21694 |
< |
2766 y(gumen)n(t)j(for)g(the)h(actual)f(densit)n(y)g(maxim)n(um)g |
30069 |
< |
(residing)g(at)g(this)-150 2861 y(midp)r(oin)n(t)36 b(v)-5 |
30070 |
< |
b(alue.)61 b(Figure)35 b(2)g(w)n(as)g(constructed)g(using)g(ice)h |
30071 |
< |
Fj(I)1849 2873 y Fi(h)-150 2956 y Fu(crystals)24 b(for)g(the)h(initial) |
30072 |
< |
g(con\014guration;)f(and)h(though)g(not)g(pic-)-150 3052 |
30073 |
< |
y(tured,)h(the)f(sim)n(ulations)f(starting)g(from)h(ice)f |
30074 |
< |
Fj(I)1325 3064 y Fi(c)1385 3052 y Fu(crystal)f(con\014g-)-150 |
30075 |
< |
3147 y(urations)j(sho)n(w)n(ed)f(similar)h(results,)g(with)h(a)g |
30076 |
< |
(liquid-phase)f(den-)-150 3243 y(sit)n(y)g(maxim)n(um)h(in)f(this)h |
30077 |
< |
(same)f(region)f(\(b)r(et)n(w)n(een)i(255)e(and)i(260)-150 |
30078 |
< |
3338 y(K\).)f(In)h(addition,)g(the)g Fj(I)627 3350 y |
30079 |
< |
Fi(c)688 3338 y Fu(crystals)e(are)g(more)h(fragile)f(than)i(the)-150 |
30080 |
< |
3434 y Fj(I)-114 3446 y Fi(h)-37 3434 y Fu(crystals,)33 |
30081 |
< |
b(leading)f(them)i(to)f(deform)g(in)n(to)f(a)h(dense)g(glassy)-150 |
30082 |
< |
3529 y(state)d(at)h(lo)n(w)n(er)d(temp)r(eratures.)45 |
30083 |
< |
b(This)31 b(resulted)f(in)g(an)h(o)n(v)n(erall)-150 3625 |
30084 |
< |
y(lo)n(w)k(temp)r(erature)g(densit)n(y)h(maxim)n(um)g(at)f(200)f(K,)i |
30085 |
< |
(but)g(they)-150 3720 y(still)i(retained)g(a)g(common)f(liquid)i(state) |
30086 |
< |
f(densit)n(y)g(maxim)n(um)-150 3816 y(with)28 b(the)g |
30087 |
< |
Fj(I)218 3828 y Fi(h)289 3816 y Fu(sim)n(ulations.)-67 |
30088 |
< |
3911 y(The)19 b(densit)n(y)g(maxim)n(um)g(for)g(SSD)h(actually)e |
30089 |
< |
(compares)g(quite)-150 4007 y(fa)n(v)n(orably)h(to)j(other)f(simple)h |
30090 |
< |
(w)n(ater)f(mo)r(dels.)35 b(Figure)21 b(3)g(sho)n(ws)g(a)-150 |
30091 |
< |
4102 y(plot)j(of)g(these)f(\014ndings)h(with)g(the)h(densit)n(y)e |
30092 |
< |
(progression)e(of)j(sev-)-150 4198 y(eral)36 b(other)g(mo)r(dels)h(and) |
30093 |
< |
f(exp)r(erimen)n(t)h(obtained)g(from)f(other)-150 4293 |
30094 |
< |
y(sources.)134 4263 y Fn(19)o({21)328 4293 y Fu(Of)26 |
21683 |
> |
1699 y(Exp)r(erimen)n(t)243 1667 y Fc(21)307 1699 y Fr(.)-150 |
21684 |
> |
1979 y Fu(lo)n(w)k(temp)r(erature)g(densit)n(y)h(maxim)n(um)g(at)f(200) |
21685 |
> |
f(K,)i(but)g(they)-150 2075 y(still)i(retained)g(a)g(common)f(liquid)i |
21686 |
> |
(state)f(densit)n(y)g(maxim)n(um)-150 2170 y(with)28 |
21687 |
> |
b(the)g Fj(I)218 2182 y Fi(h)289 2170 y Fu(sim)n(ulations.)-67 |
21688 |
> |
2266 y(The)19 b(densit)n(y)g(maxim)n(um)g(for)g(SSD)h(actually)e |
21689 |
> |
(compares)g(quite)-150 2361 y(fa)n(v)n(orably)h(to)j(other)f(simple)h |
21690 |
> |
(w)n(ater)f(mo)r(dels.)35 b(Figure)21 b(2)g(sho)n(ws)g(a)-150 |
21691 |
> |
2456 y(plot)j(of)g(these)f(\014ndings)h(with)g(the)h(densit)n(y)e |
21692 |
> |
(progression)e(of)j(sev-)-150 2552 y(eral)36 b(other)g(mo)r(dels)h(and) |
21693 |
> |
f(exp)r(erimen)n(t)h(obtained)g(from)f(other)-150 2647 |
21694 |
> |
y(sources.)134 2617 y Fn(19)o({21)328 2647 y Fu(Of)26 |
21695 |
|
b(the)g(listed)g(simple)g(w)n(ater)f(mo)r(dels,)h(SSD)h(has)-150 |
21696 |
< |
4389 y(results)d(closest)g(to)h(the)g(exp)r(erimen)n(tally)f(observ)n |
21697 |
< |
(ed)f(w)n(ater)h(den-)-150 4484 y(sit)n(y)i(maxim)n(um.)36 |
21696 |
> |
2743 y(results)d(closest)g(to)h(the)g(exp)r(erimen)n(tally)f(observ)n |
21697 |
> |
(ed)f(w)n(ater)h(den-)-150 2838 y(sit)n(y)i(maxim)n(um.)36 |
21698 |
|
b(Of)27 b(the)g(listed)f(w)n(ater)f(mo)r(dels,)i(TIP4P)e(has)h(a)-150 |
21699 |
< |
4580 y(densit)n(y)32 b(maxim)n(um)g(b)r(eha)n(vior)f(most)h(lik)n(e)g |
21700 |
< |
(that)h(seen)f(in)h(SSD.)-150 4675 y(Though)25 b(not)h(sho)n(wn,)f(it)h |
21699 |
> |
2934 y(densit)n(y)32 b(maxim)n(um)g(b)r(eha)n(vior)f(most)h(lik)n(e)g |
21700 |
> |
(that)h(seen)f(in)h(SSD.)-150 3029 y(Though)25 b(not)h(sho)n(wn,)f(it)h |
21701 |
|
(is)g(useful)g(to)f(note)h(that)g(TIP5P)e(has)h(a)-150 |
21702 |
< |
4771 y(w)n(ater)i(densit)n(y)g(maxim)n(um)g(nearly)g(iden)n(tical)g(to) |
21703 |
< |
h(exp)r(erimen)n(t.)-67 4866 y(P)n(ossibly)j(of)i(more)g(imp)r(ortance) |
21704 |
< |
f(is)h(the)h(densit)n(y)e(scaling)g(of)-150 4961 y(SSD)27 |
21702 |
> |
3125 y(w)n(ater)i(densit)n(y)g(maxim)n(um)g(nearly)g(iden)n(tical)g(to) |
21703 |
> |
h(exp)r(erimen)n(t.)-67 3220 y(P)n(ossibly)j(of)i(more)g(imp)r(ortance) |
21704 |
> |
f(is)h(the)h(densit)n(y)e(scaling)g(of)-150 3316 y(SSD)27 |
21705 |
|
b(relativ)n(e)f(to)h(other)f(common)g(mo)r(dels)h(at)f(an)n(y)g(giv)n |
21706 |
< |
(en)g(tem-)-150 5057 y(p)r(erature)31 b(\(Fig.)48 b(3\).)f(Note)32 |
21707 |
< |
b(that)f(the)h(SSD)g(mo)r(del)g(assumes)e(a)-150 5152 |
21706 |
> |
(en)g(tem-)-150 3411 y(p)r(erature)31 b(\(Fig.)48 b(2\).)f(Note)32 |
21707 |
> |
b(that)f(the)h(SSD)g(mo)r(del)g(assumes)e(a)-150 3507 |
21708 |
|
y(lo)n(w)n(er)e(densit)n(y)h(than)g(an)n(y)f(of)h(the)h(other)e(listed) |
21709 |
< |
i(mo)r(dels)f(at)g(the)-150 5248 y(same)i(pressure,)h(b)r(eha)n(vior)e |
21709 |
> |
i(mo)r(dels)f(at)g(the)-150 3602 y(same)i(pressure,)h(b)r(eha)n(vior)e |
21710 |
|
(whic)n(h)i(is)g(esp)r(ecially)f(apparen)n(t)g(at)-150 |
21711 |
< |
5343 y(temp)r(eratures)h(greater)f(than)i(300)e(K.)h(Lo)n(w)n(er)f |
21712 |
< |
(than)i(exp)r(ected)2042 -83 y(densities)d(ha)n(v)n(e)e(b)r(een)j |
21713 |
< |
(observ)n(ed)d(for)i(other)f(systems)g(with)i(the)2042 |
21714 |
< |
12 y(use)h(of)h(a)f(reaction)g(\014eld)h(for)f(long-range)e |
21715 |
< |
(electrostatic)i(in)n(ter-)2042 108 y(actions,)g(so)g(the)g(most)g(lik) |
21716 |
< |
n(ely)g(reason)e(for)i(these)g(signi\014can)n(tly)2042 |
21717 |
< |
203 y(lo)n(w)n(er)23 b(densities)h(in)h(these)g(sim)n(ulations)e(is)i |
21718 |
< |
(the)g(presence)e(of)i(the)2042 299 y(reaction)f(\014eld.)2533 |
21719 |
< |
269 y Fn(12)2629 299 y Fu(In)h(order)f(to)h(test)g(the)h(e\013ect)g(of) |
21720 |
< |
f(the)g(reaction)2042 394 y(\014eld)j(on)g(the)h(densit)n(y)f(of)g(the) |
21721 |
< |
g(systems,)g(the)h(sim)n(ulations)e(w)n(ere)2042 490 |
21722 |
< |
y(rep)r(eated)32 b(for)g(the)i(temp)r(erature)e(region)g(of)g(in)n |
21723 |
< |
(terest)h(without)2042 585 y(a)27 b(reaction)g(\014eld)h(presen)n(t.)37 |
21724 |
< |
b(The)28 b(results)f(of)h(these)g(sim)n(ulations)2042 |
21725 |
< |
681 y(are)38 b(also)g(displa)n(y)n(ed)h(in)g(\014gure)g(3.)71 |
21726 |
< |
b(Without)41 b(reaction)d(\014eld,)2042 776 y(these)26 |
21727 |
< |
b(densities)f(increase)g(considerably)f(to)i(more)f(exp)r(erimen-)2042 |
21728 |
< |
872 y(tally)43 b(reasonable)e(v)-5 b(alues,)46 b(esp)r(ecially)d |
21729 |
< |
(around)e(the)j(freezing)2042 967 y(p)r(oin)n(t)37 b(of)g(liquid)h(w)n |
21730 |
< |
(ater.)64 b(The)38 b(shap)r(e)e(of)i(the)f(curv)n(e)f(is)h(simi-)2042 |
21731 |
< |
1063 y(lar)g(to)h(the)g(curv)n(e)f(pro)r(duced)h(from)g(SSD)g(sim)n |
21732 |
< |
(ulations)g(using)2042 1158 y(reaction)e(\014eld,)k(sp)r(eci\014cally)c |
21733 |
< |
(the)i(rapidly)e(decreasing)f(densi-)2042 1254 y(ties)24 |
21711 |
> |
3698 y(temp)r(eratures)h(greater)f(than)i(300)e(K.)h(Lo)n(w)n(er)f |
21712 |
> |
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21713 |
> |
(observ)n(ed)e(for)i(other)f(systems)h(with)g(the)-150 |
21714 |
> |
3889 y(use)j(of)f(a)g(reaction)g(\014eld)h(for)f(long-range)e |
21715 |
> |
(electrostatic)i(in)n(ter-)-150 3984 y(actions,)h(so)e(the)i(most)e |
21716 |
> |
(lik)n(ely)h(reason)f(for)g(these)h(signi\014can)n(tly)-150 |
21717 |
> |
4080 y(lo)n(w)n(er)23 b(densities)h(in)h(these)g(sim)n(ulations)f(is)g |
21718 |
> |
(the)h(presence)f(of)g(the)-150 4175 y(reaction)g(\014eld.)341 |
21719 |
> |
4145 y Fn(12)437 4175 y Fu(In)h(order)f(to)h(test)h(the)f(e\013ect)h |
21720 |
> |
(of)f(the)h(reaction)-150 4271 y(\014eld)i(on)g(the)h(densit)n(y)f(of)g |
21721 |
> |
(the)h(systems,)e(the)i(sim)n(ulations)e(w)n(ere)-150 |
21722 |
> |
4366 y(rep)r(eated)32 b(for)h(the)g(temp)r(erature)f(region)g(of)h(in)n |
21723 |
> |
(terest)f(without)-150 4461 y(a)27 b(reaction)g(\014eld)h(presen)n(t.) |
21724 |
> |
37 b(The)28 b(results)g(of)f(these)h(sim)n(ulations)-150 |
21725 |
> |
4557 y(are)38 b(also)h(displa)n(y)n(ed)f(in)h(\014gure)g(2.)72 |
21726 |
> |
b(Without)40 b(reaction)e(\014eld,)-150 4652 y(these)26 |
21727 |
> |
b(densities)g(increase)e(considerably)g(to)i(more)f(exp)r(erimen-)-150 |
21728 |
> |
4748 y(tally)43 b(reasonable)e(v)-5 b(alues,)46 b(esp)r(ecially)d |
21729 |
> |
(around)f(the)h(freezing)-150 4843 y(p)r(oin)n(t)37 b(of)g(liquid)h(w)n |
21730 |
> |
(ater.)65 b(The)37 b(shap)r(e)g(of)g(the)g(curv)n(e)g(is)g(simi-)-150 |
21731 |
> |
4939 y(lar)g(to)h(the)g(curv)n(e)f(pro)r(duced)h(from)g(SSD)h(sim)n |
21732 |
> |
(ulations)e(using)-150 5034 y(reaction)f(\014eld,)k(sp)r(eci\014cally)c |
21733 |
> |
(the)i(rapidly)e(decreasing)g(densi-)-150 5130 y(ties)24 |
21734 |
|
b(at)g(higher)g(temp)r(eratures;)g(ho)n(w)n(ev)n(er,)f(a)h(sligh)n(t)g |
21735 |
< |
(shift)g(in)h(the)2042 1349 y(densit)n(y)30 b(maxim)n(um)g(lo)r |
21736 |
< |
(cation,)g(do)n(wn)f(to)h(245)f(K,)h(is)g(observ)n(ed.)2042 |
21737 |
< |
1445 y(This)21 b(is)f(probably)g(a)g(more)g(accurate)g(comparison)f(to) |
21738 |
< |
i(the)g(other)2042 1540 y(listed)f(w)n(ater)f(mo)r(dels)g(in)h(that)g |
30139 |
< |
(no)g(long)f(range)f(corrections)g(w)n(ere)2042 1636 |
30140 |
< |
y(applied)27 b(in)h(those)f(sim)n(ulations.)3079 1605 |
30141 |
< |
y Fn(19,20)2125 1731 y Fu(It)33 b(has)e(b)r(een)i(observ)n(ed)e(that)i |
30142 |
< |
(densities)f(are)f(dep)r(enden)n(t)i(on)2042 1826 y(the)j(cuto\013)h |
30143 |
< |
(radius)e(used)h(for)f(a)h(v)-5 b(ariet)n(y)35 b(of)h(w)n(ater)f(mo)r |
30144 |
< |
(dels)h(in)2042 1922 y(sim)n(ulations)g(b)r(oth)i(with)g(and)f(without) |
30145 |
< |
h(the)g(use)f(of)g(reaction)2042 2017 y(\014eld.)2217 |
30146 |
< |
1987 y Fn(12)2323 2017 y Fu(In)f(order)e(to)h(address)g(the)h(p)r |
30147 |
< |
(ossible)f(a\013ect)g(of)h(cuto\013)2042 2113 y(radius,)26 |
30148 |
< |
b(sim)n(ulations)g(w)n(ere)h(p)r(erformed)f(with)i(a)e(dip)r(olar)h |
30149 |
< |
(cuto\013)2042 2208 y(radius)j(of)g(12.0)2571 2193 y(\027)2571 |
30150 |
< |
2208 y(A)h(to)g(complimen)n(t)f(the)i(previous)d(SSD)j(sim)n(u-)2042 |
30151 |
< |
2304 y(lations,)e(all)g(p)r(erformed)g(with)h(a)f(cuto\013)g(of)g(9.0) |
30152 |
< |
3587 2289 y(\027)3587 2304 y(A.)h(All)f(the)h(re-)2042 |
30153 |
< |
2399 y(sulting)e(densities)h(o)n(v)n(erlapp)r(ed)e(within)j(error)c |
30154 |
< |
(and)j(sho)n(w)n(ed)e(no)2042 2495 y(signi\014can)n(t)21 |
30155 |
< |
b(trend)h(in)g(lo)n(w)n(er)f(or)g(higher)g(densities)i(as)e(a)h |
30156 |
< |
(function)2042 2590 y(of)33 b(cuto\013)h(radius,)h(b)r(oth)f(for)f(sim) |
30157 |
< |
n(ulations)g(with)h(and)g(without)2042 2686 y(reaction)39 |
30158 |
< |
b(\014eld.)77 b(These)40 b(results)g(indicate)h(that)g(there)f(is)g(no) |
30159 |
< |
2042 2781 y(ma)5 b(jor)26 b(b)r(ene\014t)i(in)f(c)n(ho)r(osing)f(a)h |
30160 |
< |
(longer)f(cuto\013)i(radius)e(in)i(sim)n(u-)2042 2877 |
30161 |
< |
y(lations)23 b(using)h(SSD.)h(This)f(is)g(comforting)f(in)h(that)g(the) |
30162 |
< |
h(use)f(of)g(a)2042 2972 y(longer)e(cuto\013)h(radius)f(results)h(in)g |
30163 |
< |
(a)g(near)f(doubling)h(of)g(the)h(time)2042 3068 y(required)i(to)i |
30164 |
< |
(compute)g(a)f(single)g(tra)5 b(jectory)-7 b(.)2596 3344 |
30165 |
< |
y Fo(B.)88 b(T)-7 b(ransp)r(ort)30 b(Beha)n(vior)2125 |
30166 |
< |
3557 y Fu(Of)f(imp)r(ortance)f(in)h(these)f(t)n(yp)r(es)h(of)g(studies) |
30167 |
< |
f(are)g(the)h(trans-)2042 3653 y(p)r(ort)44 b(prop)r(erties)f(of)h(the) |
30168 |
< |
g(particles)f(and)h(ho)n(w)f(they)h(c)n(hange)2042 3748 |
30169 |
< |
y(when)29 b(altering)f(the)h(en)n(vironmen)n(tal)e(conditions.)41 |
30170 |
< |
b(In)29 b(order)e(to)2042 3844 y(prob)r(e)34 b(transp)r(ort,)i(constan) |
30171 |
< |
n(t)d(energy)h(sim)n(ulations)g(w)n(ere)g(p)r(er-)2042 |
30172 |
< |
3939 y(formed)27 b(ab)r(out)g(the)h(a)n(v)n(erage)c(densit)n(y)j(unco)n |
30173 |
< |
(v)n(ered)f(b)n(y)h(the)h(con-)2042 4035 y(stan)n(t)21 |
30174 |
< |
b(pressure)g(sim)n(ulations.)34 b(Sim)n(ulations)22 b(started)f(with)h |
30175 |
< |
(ran-)2042 4130 y(domized)32 b(v)n(elo)r(cities)f(and)h(underw)n(en)n |
30176 |
< |
(t)g(50)f(ps)h(of)h(temp)r(erature)2042 4226 y(scaling)25 |
30177 |
< |
b(and)h(50)f(ps)h(of)g(constan)n(t)f(energy)g(equilibration)g(b)r |
30178 |
< |
(efore)2042 4321 y(obtaining)32 b(a)h(200)e(ps)i(tra)5 |
30179 |
< |
b(jectory)-7 b(.)52 b(Di\013usion)33 b(constan)n(ts)f(w)n(ere)2042 |
30180 |
< |
4417 y(calculated)27 b(via)h(ro)r(ot-mean)f(square)f(deviation)i |
30181 |
< |
(analysis.)37 b(The)2042 4512 y(a)n(v)n(eraged)e(results)i(from)h(5)f |
30182 |
< |
(sets)h(of)f(these)h(NVE)g(sim)n(ulations)2042 4608 y(is)29 |
30183 |
< |
b(displa)n(y)n(ed)f(in)i(\014gure)f(4,)g(alongside)f(exp)r(erimen)n |
30184 |
< |
(tal,)h(SPC/E,)2042 4703 y(and)e(TIP5P)f(results.)2735 |
30185 |
< |
4673 y Fn(4,20,22,23)2125 4799 y Fu(The)38 b(observ)n(ed)e(v)-5 |
30186 |
< |
b(alues)37 b(for)g(the)h(di\013usion)g(constan)n(t)f(p)r(oin)n(t)2042 |
30187 |
< |
4894 y(out)45 b(one)g(of)g(the)h(strengths)e(of)h(the)h(SSD)g(mo)r |
30188 |
< |
(del.)90 b(Of)45 b(the)2042 4990 y(three)39 b(exp)r(erimen)n(tal)g(mo)r |
30189 |
< |
(dels)g(sho)n(wn,)j(the)e(SSD)g(mo)r(del)g(has)2042 5085 |
30190 |
< |
y(the)23 b(most)g(accurate)f(depiction)i(of)f(the)g(di\013usion)h |
30191 |
< |
(trend)f(seen)g(in)2042 5180 y(exp)r(erimen)n(t)i(in)g(b)r(oth)h(the)g |
30192 |
< |
(sup)r(erco)r(oled)e(and)h(normal)f(regimes.)2042 5276 |
30193 |
< |
y(SPC/E)19 b(do)r(es)h(a)g(resp)r(ectable)f(job)h(b)n(y)g(getting)g |
30194 |
< |
(similar)g(v)-5 b(alues)20 b(as)2042 5371 y(SSD)28 b(and)f(exp)r |
30195 |
< |
(erimen)n(t)h(around)e(290)g(K;)h(ho)n(w)n(ev)n(er,)f(it)i(deviates)p |
30196 |
< |
eop |
30197 |
< |
%%Page: 5 5 |
30198 |
< |
5 4 bop 4043 -299 a Fu(5)-129 -166 y |
21735 |
> |
(shift)h(in)f(the)-150 5225 y(densit)n(y)30 b(maxim)n(um)g(lo)r |
21736 |
> |
(cation,)g(do)n(wn)g(to)f(245)g(K,)h(is)g(observ)n(ed.)-150 |
21737 |
> |
5321 y(This)21 b(is)f(probably)g(a)h(more)f(accurate)f(comparison)g(to) |
21738 |
> |
i(the)g(other)2063 -166 y |
21739 |
|
gsave currentpoint currentpoint translate -90 neg rotate neg exch |
21740 |
|
neg exch translate |
21741 |
< |
-129 -166 a @beginspecial |
21742 |
< |
104 @llx 85 @lly 556 @urx 674 @ury 1842 @rwi @setspecial |
21741 |
> |
2063 -166 a @beginspecial 104 |
21742 |
> |
@llx 85 @lly 556 @urx 674 @ury 1842 @rwi @setspecial |
21743 |
|
%%BeginDocument: betterDiffuse.epsi |
21744 |
|
%!PS-Adobe-2.0 EPSF-1.2 |
21745 |
|
%%Title: betterDiffuse.ps |
29716 |
|
%%EOF |
29717 |
|
|
29718 |
|
%%EndDocument |
29719 |
< |
@endspecial 1406 -166 a |
29719 |
> |
@endspecial 3598 -166 a |
29720 |
|
currentpoint grestore moveto |
29721 |
< |
1406 -166 a -150 1513 a Fr(FIG.)22 |
29722 |
< |
b(4:)33 b(Av)n(erage)22 b(di\013usion)f(co)r(e\016cien)n(t)i(o)n(v)n |
29723 |
< |
(er)e(increasing)i(temp)r(era-)-150 1600 y(ture)c(for)i(SSD,)e(SPC/E) |
29724 |
< |
543 1568 y Fc(20)609 1600 y Fr(,)i(TIP5P)876 1568 y Fc(4)911 |
29725 |
< |
1600 y Fr(,)g(and)f(Exp)r(erimen)n(tal)f(data)g(from)-150 |
29726 |
< |
1687 y(Gillen)27 b Fs(et)h(al.)248 1655 y Fc(22)312 1687 |
29727 |
< |
y Fr(,)e(and)g(from)f(Mills)853 1655 y Fc(23)920 1687 |
29728 |
< |
y Fr(.)-150 1967 y Fu(at)f(b)r(oth)i(higher)d(and)i(lo)n(w)n(er)e(temp) |
29729 |
< |
r(eratures,)i(failing)f(to)g(predict)-150 2063 y(the)33 |
29730 |
< |
b(exp)r(erimen)n(tal)f(trend.)51 b(TIP5P)31 b(and)h(SSD)h(b)r(oth)g |
29731 |
< |
(start)e(o\013)-150 2158 y(lo)n(w)j(at)h(the)h(colder)e(temp)r |
29732 |
< |
(eratures)g(and)h(tend)g(to)g(di\013use)h(to)r(o)-150 |
29733 |
< |
2254 y(rapidly)d(at)g(the)g(higher)g(temp)r(eratures.)53 |
29734 |
< |
b(This)34 b(t)n(yp)r(e)f(of)g(trend)-150 2349 y(at)e(the)g(higher)g |
29735 |
< |
(temp)r(eratures)f(is)h(not)g(surprising)e(in)j(that)f(the)-150 |
29736 |
< |
2445 y(densities)c(of)h(b)r(oth)g(TIP5P)e(and)h(SSD)h(are)f(lo)n(w)n |
29737 |
< |
(er)e(than)j(exp)r(eri-)-150 2540 y(men)n(tal)d(w)n(ater)g(at)g(temp)r |
29738 |
< |
(eratures)g(higher)g(than)h(ro)r(om)e(temp)r(er-)-150 |
29739 |
< |
2635 y(ature.)34 b(When)20 b(calculating)f(the)h(di\013usion)g(co)r |
29740 |
< |
(e\016cien)n(ts)f(for)h(SSD)-150 2731 y(at)32 b(exp)r(erimen)n(tal)f |
29741 |
< |
(densities,)i(the)f(resulting)g(v)-5 b(alues)31 b(fall)h(more)-150 |
29742 |
< |
2826 y(in)24 b(line)h(with)f(exp)r(erimen)n(t)g(at)g(these)g(temp)r |
29743 |
< |
(eratures,)g(alb)r(eit)g(not)-150 2922 y(at)g(standard)e(pressure.)35 |
29744 |
< |
b(Results)23 b(under)h(these)g(conditions)f(can)-150 |
29745 |
< |
3017 y(b)r(e)28 b(found)g(later)f(in)h(this)g(pap)r(er.)-15 |
29746 |
< |
3294 y Fo(C.)88 b(Structural)32 b(Changes)d(and)h(Characterization)-67 |
29747 |
< |
3507 y Fu(By)e(starting)f(the)h(sim)n(ulations)f(from)g(the)i |
29748 |
< |
(crystalline)e(state,)-150 3603 y(the)f(melting)h(transition)e(and)h |
29749 |
< |
(the)g(ice)g(structure)f(can)h(b)r(e)g(stud-)-150 3698 |
29750 |
< |
y(ied)20 b(along)f(with)h(the)h(liquid)f(phase)g(b)r(eha)n(vior)e(b)r |
29751 |
< |
(ey)n(ond)i(the)g(melt-)-150 3794 y(ing)27 b(p)r(oin)n(t.)37 |
29752 |
< |
b(T)-7 b(o)26 b(lo)r(cate)h(the)g(melting)g(transition,)g(the)g |
29753 |
< |
(constan)n(t)-150 3889 y(pressure)22 b(heat)i(capacit)n(y)e(\(C)766 |
29754 |
< |
3901 y Fn(p)807 3889 y Fu(\))i(w)n(as)e(monitored)h(in)h(eac)n(h)f(of)g |
29755 |
< |
(the)-150 3984 y(sim)n(ulations.)34 b(In)22 b(the)g(melting)f(sim)n |
29756 |
< |
(ulations)g(of)h(the)g(1024)d(parti-)-150 4080 y(cle)i(ice)g |
29757 |
< |
Fj(I)122 4092 y Fi(h)187 4080 y Fu(sim)n(ulations,)g(a)g(large)e(spik)n |
29758 |
< |
(e)i(in)g(C)1252 4092 y Fn(p)1314 4080 y Fu(o)r(ccurs)f(at)h(245)f(K,) |
29759 |
< |
-150 4175 y(indicating)33 b(a)g(\014rst)g(order)f(phase)g(transition)h |
29760 |
< |
(for)g(the)g(melting)-150 4271 y(of)h(these)g(ice)f(crystals.)54 |
29761 |
< |
b(When)35 b(the)f(reaction)f(\014eld)h(is)f(turned)-150 |
29762 |
< |
4366 y(o\013,)22 b(the)g(melting)f(transition)f(o)r(ccurs)g(at)h(235)f |
29763 |
< |
(K.)h(These)f(melting)-150 4462 y(transitions)25 b(are)h(considerably)e |
29764 |
< |
(lo)n(w)n(er)h(than)h(the)h(exp)r(erimen)n(tal)-150 4557 |
29765 |
< |
y(v)-5 b(alue,)31 b(but)g(this)g(is)f(not)g(surprising)f(in)i(that)g |
29766 |
< |
(SSD)g(is)f(a)g(simple)-150 4653 y(rigid)d(b)r(o)r(dy)h(mo)r(del)g |
29767 |
< |
(with)g(a)f(\014xed)g(dip)r(ole.)-67 4748 y(Additional)71 |
29768 |
< |
b(analyses)e(for)i(understanding)f(the)h(melt-)-150 4844 |
29721 |
> |
3598 -166 a 2042 1513 a Fr(FIG.)h(3:)33 |
29722 |
> |
b(Av)n(erage)21 b(di\013usion)h(co)r(e\016cien)n(t)h(o)n(v)n(er)e |
29723 |
> |
(increasing)i(temp)r(era-)2042 1600 y(ture)c(for)h(SSD,)f(SPC/E)2734 |
29724 |
> |
1568 y Fc(20)2800 1600 y Fr(,)i(TIP5P)3067 1568 y Fc(4)3103 |
29725 |
> |
1600 y Fr(,)g(and)e(Exp)r(erimen)n(tal)g(data)h(from)2042 |
29726 |
> |
1687 y(Gillen)26 b Fs(et)j(al.)2440 1655 y Fc(22)2504 |
29727 |
> |
1687 y Fr(,)d(and)f(from)h(Mills)3045 1655 y Fc(23)3111 |
29728 |
> |
1687 y Fr(.)2042 1967 y Fu(listed)20 b(w)n(ater)f(mo)r(dels)g(in)h |
29729 |
> |
(that)g(no)g(long)f(range)f(corrections)g(w)n(ere)2042 |
29730 |
> |
2063 y(applied)27 b(in)h(those)f(sim)n(ulations.)3079 |
29731 |
> |
2032 y Fn(19,20)2125 2158 y Fu(It)33 b(has)e(b)r(een)i(observ)n(ed)e |
29732 |
> |
(that)i(densities)f(are)f(dep)r(enden)n(t)i(on)2042 2254 |
29733 |
> |
y(the)j(cuto\013)h(radius)e(used)h(for)f(a)h(v)-5 b(ariet)n(y)35 |
29734 |
> |
b(of)h(w)n(ater)f(mo)r(dels)h(in)2042 2349 y(sim)n(ulations)g(b)r(oth)i |
29735 |
> |
(with)g(and)f(without)h(the)g(use)f(of)g(reaction)2042 |
29736 |
> |
2445 y(\014eld.)2217 2414 y Fn(12)2323 2445 y Fu(In)f(order)e(to)h |
29737 |
> |
(address)g(the)h(p)r(ossible)f(a\013ect)g(of)h(cuto\013)2042 |
29738 |
> |
2540 y(radius,)26 b(sim)n(ulations)g(w)n(ere)h(p)r(erformed)f(with)i(a) |
29739 |
> |
e(dip)r(olar)h(cuto\013)2042 2635 y(radius)j(of)g(12.0)2571 |
29740 |
> |
2620 y(\027)2571 2635 y(A)h(to)g(complimen)n(t)f(the)i(previous)d(SSD)j |
29741 |
> |
(sim)n(u-)2042 2731 y(lations,)e(all)g(p)r(erformed)g(with)h(a)f |
29742 |
> |
(cuto\013)g(of)g(9.0)3587 2716 y(\027)3587 2731 y(A.)h(All)f(the)h(re-) |
29743 |
> |
2042 2826 y(sulting)e(densities)h(o)n(v)n(erlapp)r(ed)e(within)j(error) |
29744 |
> |
c(and)j(sho)n(w)n(ed)e(no)2042 2922 y(signi\014can)n(t)21 |
29745 |
> |
b(trend)h(in)g(lo)n(w)n(er)f(or)g(higher)g(densities)i(as)e(a)h |
29746 |
> |
(function)2042 3017 y(of)33 b(cuto\013)h(radius,)h(b)r(oth)f(for)f(sim) |
29747 |
> |
n(ulations)g(with)h(and)g(without)2042 3113 y(reaction)39 |
29748 |
> |
b(\014eld.)77 b(These)40 b(results)g(indicate)h(that)g(there)f(is)g(no) |
29749 |
> |
2042 3208 y(ma)5 b(jor)26 b(b)r(ene\014t)i(in)f(c)n(ho)r(osing)f(a)h |
29750 |
> |
(longer)f(cuto\013)i(radius)e(in)i(sim)n(u-)2042 3304 |
29751 |
> |
y(lations)23 b(using)h(SSD.)h(This)f(is)g(comforting)f(in)h(that)g(the) |
29752 |
> |
h(use)f(of)g(a)2042 3399 y(longer)e(cuto\013)h(radius)f(results)h(in)g |
29753 |
> |
(a)g(near)f(doubling)h(of)g(the)h(time)2042 3495 y(required)i(to)i |
29754 |
> |
(compute)g(a)f(single)g(tra)5 b(jectory)-7 b(.)2596 3771 |
29755 |
> |
y Fo(B.)88 b(T)-7 b(ransp)r(ort)30 b(Beha)n(vior)2125 |
29756 |
> |
3984 y Fu(Of)f(imp)r(ortance)f(in)h(these)f(t)n(yp)r(es)h(of)g(studies) |
29757 |
> |
f(are)g(the)h(trans-)2042 4080 y(p)r(ort)44 b(prop)r(erties)f(of)h(the) |
29758 |
> |
g(particles)f(and)h(ho)n(w)f(they)h(c)n(hange)2042 4175 |
29759 |
> |
y(when)29 b(altering)f(the)h(en)n(vironmen)n(tal)e(conditions.)41 |
29760 |
> |
b(In)29 b(order)e(to)2042 4271 y(prob)r(e)34 b(transp)r(ort,)i(constan) |
29761 |
> |
n(t)d(energy)h(sim)n(ulations)g(w)n(ere)g(p)r(er-)2042 |
29762 |
> |
4366 y(formed)27 b(ab)r(out)g(the)h(a)n(v)n(erage)c(densit)n(y)j(unco)n |
29763 |
> |
(v)n(ered)f(b)n(y)h(the)h(con-)2042 4462 y(stan)n(t)21 |
29764 |
> |
b(pressure)g(sim)n(ulations.)34 b(Sim)n(ulations)22 b(started)f(with)h |
29765 |
> |
(ran-)2042 4557 y(domized)32 b(v)n(elo)r(cities)f(and)h(underw)n(en)n |
29766 |
> |
(t)g(50)f(ps)h(of)h(temp)r(erature)2042 4653 y(scaling)25 |
29767 |
> |
b(and)h(50)f(ps)h(of)g(constan)n(t)f(energy)g(equilibration)g(b)r |
29768 |
> |
(efore)2042 4748 y(obtaining)32 b(a)h(200)e(ps)i(tra)5 |
29769 |
> |
b(jectory)-7 b(.)52 b(Di\013usion)33 b(constan)n(ts)f(w)n(ere)2042 |
29770 |
> |
4844 y(calculated)27 b(via)h(ro)r(ot-mean)f(square)f(deviation)i |
29771 |
> |
(analysis.)37 b(The)2042 4939 y(a)n(v)n(eraged)e(results)i(from)h(5)f |
29772 |
> |
(sets)h(of)f(these)h(NVE)g(sim)n(ulations)2042 5035 y(is)29 |
29773 |
> |
b(displa)n(y)n(ed)f(in)i(\014gure)f(3,)g(alongside)f(exp)r(erimen)n |
29774 |
> |
(tal,)h(SPC/E,)2042 5130 y(and)e(TIP5P)f(results.)2735 |
29775 |
> |
5100 y Fn(4,20,22,23)2125 5226 y Fu(The)38 b(observ)n(ed)e(v)-5 |
29776 |
> |
b(alues)37 b(for)g(the)h(di\013usion)g(constan)n(t)f(p)r(oin)n(t)2042 |
29777 |
> |
5321 y(out)45 b(one)g(of)g(the)h(strengths)e(of)h(the)h(SSD)g(mo)r |
29778 |
> |
(del.)90 b(Of)45 b(the)2042 5417 y(three)39 b(exp)r(erimen)n(tal)g(mo)r |
29779 |
> |
(dels)g(sho)n(wn,)j(the)e(SSD)g(mo)r(del)g(has)p eop |
29780 |
> |
%%Page: 5 5 |
29781 |
> |
5 4 bop 4043 -299 a Fu(5)-150 -83 y(the)24 b(most)f(accurate)e |
29782 |
> |
(depiction)j(of)f(the)h(di\013usion)f(trend)g(seen)g(in)-150 |
29783 |
> |
12 y(exp)r(erimen)n(t)i(in)h(b)r(oth)f(the)h(sup)r(erco)r(oled)e(and)h |
29784 |
> |
(normal)f(regimes.)-150 108 y(SPC/E)19 b(do)r(es)h(a)g(resp)r(ectable)f |
29785 |
> |
(job)i(b)n(y)f(getting)g(similar)f(v)-5 b(alues)20 b(as)-150 |
29786 |
> |
203 y(SSD)28 b(and)g(exp)r(erimen)n(t)f(around)f(290)g(K;)i(ho)n(w)n |
29787 |
> |
(ev)n(er,)d(it)j(deviates)-150 299 y(at)c(b)r(oth)i(higher)d(and)i(lo)n |
29788 |
> |
(w)n(er)e(temp)r(eratures,)i(failing)f(to)g(predict)-150 |
29789 |
> |
394 y(the)33 b(exp)r(erimen)n(tal)f(trend.)51 b(TIP5P)31 |
29790 |
> |
b(and)h(SSD)h(b)r(oth)g(start)e(o\013)-150 490 y(lo)n(w)j(at)h(the)h |
29791 |
> |
(colder)e(temp)r(eratures)g(and)h(tend)g(to)g(di\013use)h(to)r(o)-150 |
29792 |
> |
585 y(rapidly)d(at)g(the)g(higher)g(temp)r(eratures.)53 |
29793 |
> |
b(This)34 b(t)n(yp)r(e)f(of)g(trend)-150 681 y(at)e(the)g(higher)g |
29794 |
> |
(temp)r(eratures)f(is)h(not)g(surprising)e(in)j(that)f(the)-150 |
29795 |
> |
776 y(densities)c(of)h(b)r(oth)g(TIP5P)e(and)h(SSD)h(are)f(lo)n(w)n(er) |
29796 |
> |
e(than)j(exp)r(eri-)-150 872 y(men)n(tal)d(w)n(ater)g(at)g(temp)r |
29797 |
> |
(eratures)g(higher)g(than)h(ro)r(om)e(temp)r(er-)-150 |
29798 |
> |
967 y(ature.)34 b(When)20 b(calculating)f(the)h(di\013usion)g(co)r |
29799 |
> |
(e\016cien)n(ts)f(for)h(SSD)-150 1063 y(at)32 b(exp)r(erimen)n(tal)f |
29800 |
> |
(densities,)i(the)f(resulting)g(v)-5 b(alues)31 b(fall)h(more)-150 |
29801 |
> |
1158 y(in)24 b(line)h(with)f(exp)r(erimen)n(t)g(at)g(these)g(temp)r |
29802 |
> |
(eratures,)g(alb)r(eit)g(not)-150 1254 y(at)g(standard)e(pressure.)35 |
29803 |
> |
b(Results)23 b(under)h(these)g(conditions)f(can)-150 |
29804 |
> |
1349 y(b)r(e)28 b(found)g(later)f(in)h(this)g(pap)r(er.)-15 |
29805 |
> |
1625 y Fo(C.)88 b(Structural)32 b(Changes)d(and)h(Characterization)-67 |
29806 |
> |
1839 y Fu(By)e(starting)f(the)h(sim)n(ulations)f(from)g(the)i |
29807 |
> |
(crystalline)e(state,)-150 1934 y(the)f(melting)h(transition)e(and)h |
29808 |
> |
(the)g(ice)g(structure)f(can)h(b)r(e)g(stud-)-150 2030 |
29809 |
> |
y(ied)20 b(along)f(with)h(the)h(liquid)f(phase)g(b)r(eha)n(vior)e(b)r |
29810 |
> |
(ey)n(ond)i(the)g(melt-)-150 2125 y(ing)27 b(p)r(oin)n(t.)37 |
29811 |
> |
b(T)-7 b(o)26 b(lo)r(cate)h(the)g(melting)g(transition,)g(the)g |
29812 |
> |
(constan)n(t)-150 2221 y(pressure)22 b(heat)i(capacit)n(y)e(\(C)766 |
29813 |
> |
2233 y Fn(p)807 2221 y Fu(\))i(w)n(as)e(monitored)h(in)h(eac)n(h)f(of)g |
29814 |
> |
(the)-150 2316 y(sim)n(ulations.)34 b(In)22 b(the)g(melting)f(sim)n |
29815 |
> |
(ulations)g(of)h(the)g(1024)d(parti-)-150 2412 y(cle)i(ice)g |
29816 |
> |
Fj(I)122 2424 y Fi(h)187 2412 y Fu(sim)n(ulations,)g(a)g(large)e(spik)n |
29817 |
> |
(e)i(in)g(C)1252 2424 y Fn(p)1314 2412 y Fu(o)r(ccurs)f(at)h(245)f(K,) |
29818 |
> |
-150 2507 y(indicating)33 b(a)g(\014rst)g(order)f(phase)g(transition)h |
29819 |
> |
(for)g(the)g(melting)-150 2603 y(of)h(these)g(ice)f(crystals.)54 |
29820 |
> |
b(When)35 b(the)f(reaction)f(\014eld)h(is)f(turned)-150 |
29821 |
> |
2698 y(o\013,)22 b(the)g(melting)f(transition)f(o)r(ccurs)g(at)h(235)f |
29822 |
> |
(K.)h(These)f(melting)-150 2794 y(transitions)25 b(are)h(considerably)e |
29823 |
> |
(lo)n(w)n(er)h(than)h(the)h(exp)r(erimen)n(tal)-150 2889 |
29824 |
> |
y(v)-5 b(alue,)31 b(but)g(this)g(is)f(not)g(surprising)f(in)i(that)g |
29825 |
> |
(SSD)g(is)f(a)g(simple)-150 2985 y(rigid)d(b)r(o)r(dy)h(mo)r(del)g |
29826 |
> |
(with)g(a)f(\014xed)g(dip)r(ole.)-67 3080 y(Additional)71 |
29827 |
> |
b(analyses)e(for)i(understanding)f(the)h(melt-)-150 3175 |
29828 |
|
y(ing)48 b(phase-transition)e(pro)r(cess)h(w)n(ere)g(p)r(erformed)h |
29829 |
< |
(via)g(t)n(w)n(o-)-150 4939 y(dimensional)26 b(structure)h(and)f(dip)r |
29830 |
< |
(ole)h(angle)f(correlations.)34 b(Ex-)-150 5035 y(pressions)26 |
29831 |
< |
b(for)h(the)h(correlations)e(are)g(as)h(follo)n(ws:)2059 |
29832 |
< |
1788 y @beginspecial 0 @llx 0 @lly 965 @urx 939 @ury |
29833 |
< |
2409 @rwi @setspecial |
29829 |
> |
(via)g(t)n(w)n(o-)-150 3271 y(dimensional)26 b(structure)h(and)f(dip)r |
29830 |
> |
(ole)h(angle)f(correlations.)34 b(Ex-)-150 3366 y(pressions)26 |
29831 |
> |
b(for)h(the)h(correlations)e(are)g(as)h(follo)n(ws:)-67 |
29832 |
> |
3665 y Fj(g)-27 3677 y Fn(AB)72 3665 y Fu(\()p Fj(r)n(;)14 |
29833 |
> |
b Fu(cos)g Fj(\022)r Fu(\))23 b(=)172 3784 y Fj(V)p 87 |
29834 |
> |
3821 238 4 v 87 3897 a(N)154 3909 y Fn(A)207 3897 y Fj(N)274 |
29835 |
> |
3909 y Fn(B)334 3840 y Ff(h)366 3761 y Fg(X)367 3939 |
29836 |
> |
y Fi(i)p Ft(2)p Fn(A)501 3761 y Fg(X)500 3939 y Fi(j)s |
29837 |
> |
Ft(2)p Fn(B)636 3840 y Fj(\016)s Fu(\(cos)13 b Fj(\022)21 |
29838 |
> |
b Ff(\000)d Fu(cos)13 b Fj(\022)1140 3852 y Fi(ij)1198 |
29839 |
> |
3840 y Fu(\))p Fj(\016)s Fu(\()p Fj(r)22 b Ff(\000)c(j)p |
29840 |
> |
Fh(r)1506 3852 y Fi(ij)1565 3840 y Ff(j)p Fu(\))p Ff(i)28 |
29841 |
> |
b Fj(;)83 b Fu(\(8\))-67 4225 y Fj(g)-27 4237 y Fn(AB)72 |
29842 |
> |
4225 y Fu(\()p Fj(r)n(;)14 b Fu(cos)g Fj(!)s Fu(\))23 |
29843 |
> |
b(=)146 4344 y Fj(V)p 61 4381 V 61 4457 a(N)128 4469 |
29844 |
> |
y Fn(A)180 4457 y Fj(N)247 4469 y Fn(B)308 4400 y Ff(h)340 |
29845 |
> |
4321 y Fg(X)341 4499 y Fi(i)p Ft(2)p Fn(A)475 4321 y |
29846 |
> |
Fg(X)474 4499 y Fi(j)s Ft(2)p Fn(B)610 4400 y Fj(\016)s |
29847 |
> |
Fu(\(cos)13 b Fj(!)21 b Ff(\000)d Fu(cos)13 b Fj(!)1140 |
29848 |
> |
4412 y Fi(ij)1198 4400 y Fu(\))p Fj(\016)s Fu(\()p Fj(r)22 |
29849 |
> |
b Ff(\000)c(j)p Fh(r)1506 4412 y Fi(ij)1565 4400 y Ff(j)p |
29850 |
> |
Fu(\))p Ff(i)28 b Fj(;)83 b Fu(\(9\))-150 4668 y(where)19 |
29851 |
> |
b Fj(\022)j Fu(and)d Fj(!)j Fu(refer)c(to)i(the)f(angles)g(sho)n(wn)f |
29852 |
> |
(in)i(the)g(ab)r(o)n(v)n(e)e(illus-)-150 4763 y(tration.)36 |
29853 |
> |
b(By)26 b(binning)g(o)n(v)n(er)f(b)r(oth)i(distance)f(and)g(the)h |
29854 |
> |
(cosine)e(of)-150 4858 y(the)31 b(desired)g(angle)f(b)r(et)n(w)n(een)h |
29855 |
> |
(the)h(t)n(w)n(o)e(dip)r(oles,)i(the)g(g\()p Fm(r)9 b |
29856 |
> |
Fu(\))31 b(can)-150 4954 y(b)r(e)38 b(dissected)f(to)f(determine)i(the) |
29857 |
> |
f(common)g(dip)r(ole)g(arrange-)-150 5049 y(men)n(ts)29 |
29858 |
> |
b(that)g(constitute)g(the)h(p)r(eaks)e(and)h(troughs.)40 |
29859 |
> |
b(F)-7 b(rames)28 b(A)-150 5145 y(and)d(B)h(of)f(\014gure)g(4)g(sho)n |
29860 |
> |
(w)g(a)g(relativ)n(ely)f(crystalline)h(state)g(of)h(an)-150 |
29861 |
> |
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29862 |
> |
b(The)36 b(\014rst)g(p)r(eak)g(of)g(the)g(g\()p Fm(r)9 |
29863 |
> |
b Fu(\))36 b(primarily)-150 5336 y(consists)23 b(of)h(the)g(preferred)f |
29864 |
> |
(h)n(ydrogen)f(b)r(onding)i(arrangemen)n(ts)-150 5431 |
29865 |
> |
y(as)i(dictated)i(b)n(y)e(the)i(tetrahedral)e(stic)n(ky)g(p)r(oten)n |
29866 |
> |
(tial,)h(one)g(p)r(eak)2059 1788 y @beginspecial 0 @llx |
29867 |
> |
0 @lly 965 @urx 939 @ury 2409 @rwi @setspecial |
29868 |
|
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29869 |
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29870 |
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64952 |
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64953 |
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64954 |
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64955 |
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@endspecial 2042 1958 a Fr(FIG.)g(5:)39 b(Con)n(tour)27 |
64955 |
> |
@endspecial 2042 1958 a Fr(FIG.)g(4:)39 b(Con)n(tour)27 |
64956 |
|
b(plots)h(of)g(2D)g(angular)g(g\()p Fq(r)r Fr(\)'s)g(for)g(512)g(SSD)e |
64957 |
|
(sys-)2042 2045 y(tems)h(at)h(100)h(K)e(\(A)g(&)h(B\))g(and)f(300)i(K)e |
64958 |
|
(\(C)h(&)g(D\).)f(Con)n(tour)i(colors)2042 2132 y(are)i(in)n(v)n(erted) |
71090 |
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71091 |
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71092 |
|
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71093 |
< |
@endspecial 2042 3428 a(FIG.)31 b(6:)46 b(Tw)n(o)32 |
71093 |
> |
@endspecial 2042 3428 a(FIG.)31 b(5:)46 b(Tw)n(o)32 |
71094 |
|
b(dimensional)f(illustration)i(of)f(the)f(angles)h(in)n(v)n(olv)n(ed) |
71095 |
|
2042 3515 y(in)25 b(the)h(correlations)h(observ)n(ed)f(in)f(\014gure)h |
71096 |
< |
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71097 |
< |
Fj(r)n(;)14 b Fu(cos)f Fj(\022)r Fu(\))24 b(=)2364 4118 |
71098 |
< |
y Fj(V)p 2278 4155 238 4 v 2278 4231 a(N)2345 4243 y |
71099 |
< |
Fn(A)2398 4231 y Fj(N)2465 4243 y Fn(B)2526 4174 y Ff(h)2558 |
71100 |
< |
4095 y Fg(X)2559 4273 y Fi(i)p Ft(2)p Fn(A)2693 4095 |
71101 |
< |
y Fg(X)2692 4273 y Fi(j)s Ft(2)p Fn(B)2827 4174 y Fj(\016)s |
71102 |
< |
Fu(\(cos)14 b Fj(\022)20 b Ff(\000)f Fu(cos)13 b Fj(\022)3332 |
71103 |
< |
4186 y Fi(ij)3390 4174 y Fu(\))p Fj(\016)s Fu(\()p Fj(r)22 |
71104 |
< |
b Ff(\000)c(j)p Fh(r)3698 4186 y Fi(ij)3757 4174 y Ff(j)p |
71105 |
< |
Fu(\))p Ff(i)28 b Fj(;)83 b Fu(\(8\))2125 4559 y Fj(g)2165 |
71106 |
< |
4571 y Fn(AB)2264 4559 y Fu(\()p Fj(r)n(;)14 b Fu(cos)f |
71107 |
< |
Fj(!)s Fu(\))23 b(=)2338 4677 y Fj(V)p 2252 4714 V 2252 |
71108 |
< |
4790 a(N)2319 4802 y Fn(A)2372 4790 y Fj(N)2439 4802 |
71109 |
< |
y Fn(B)2499 4733 y Ff(h)2531 4655 y Fg(X)2532 4833 y |
71110 |
< |
Fi(i)p Ft(2)p Fn(A)2667 4655 y Fg(X)2666 4833 y Fi(j)s |
71111 |
< |
Ft(2)p Fn(B)2801 4733 y Fj(\016)s Fu(\(cos)14 b Fj(!)21 |
71112 |
< |
b Ff(\000)d Fu(cos)13 b Fj(!)3332 4745 y Fi(ij)3390 4733 |
71113 |
< |
y Fu(\))p Fj(\016)s Fu(\()p Fj(r)22 b Ff(\000)c(j)p Fh(r)3698 |
71114 |
< |
4745 y Fi(ij)3757 4733 y Ff(j)p Fu(\))p Ff(i)28 b Fj(;)83 |
71115 |
< |
b Fu(\(9\))2042 5001 y(where)19 b Fj(\022)i Fu(and)f |
71116 |
< |
Fj(!)i Fu(refer)c(to)h(the)h(angles)e(sho)n(wn)h(in)h(the)f(ab)r(o)n(v) |
71117 |
< |
n(e)f(illus-)2042 5097 y(tration.)36 b(By)26 b(binning)g(o)n(v)n(er)f |
71118 |
< |
(b)r(oth)i(distance)f(and)g(the)h(cosine)e(of)2042 5192 |
71119 |
< |
y(the)31 b(desired)g(angle)f(b)r(et)n(w)n(een)h(the)h(t)n(w)n(o)e(dip)r |
71120 |
< |
(oles,)i(the)f(g\()p Fm(r)9 b Fu(\))32 b(can)2042 5288 |
71121 |
< |
y(b)r(e)37 b(dissected)g(to)g(determine)g(the)h(common)f(dip)r(ole)g |
79489 |
< |
(arrange-)2042 5383 y(men)n(ts)29 b(that)g(constitute)g(the)h(p)r(eaks) |
79490 |
< |
e(and)h(troughs.)40 b(F)-7 b(rames)28 b(A)2042 5479 y(and)d(B)h(of)f |
79491 |
< |
(\014gure)g(5)g(sho)n(w)g(a)g(relativ)n(ely)f(crystalline)h(state)g(of) |
79492 |
< |
g(an)p eop |
71096 |
> |
(4.)2042 3796 y Fu(for)k(the)i(donating)e(and)h(the)g(other)f(for)h |
71097 |
> |
(the)g(accepting)g(h)n(ydro-)2042 3891 y(gen)39 b(b)r(onds.)73 |
71098 |
> |
b(Due)40 b(to)g(the)g(high)f(degree)g(of)h(crystallinit)n(y)e(of)2042 |
71099 |
> |
3987 y(the)e(sample,)i(the)f(second)e(and)h(third)g(solv)-5 |
71100 |
> |
b(ation)35 b(shells)h(sho)n(w)2042 4082 y(a)30 b(rep)r(eated)h(p)r(eak) |
71101 |
> |
f(arrangemen)n(t)f(whic)n(h)h(deca)n(ys)g(at)h(distances)2042 |
71102 |
> |
4178 y(around)19 b(the)j(fourth)e(solv)-5 b(ation)20 |
71103 |
> |
b(shell,)i(near)e(the)h(imp)r(osed)g(cuto\013)2042 4273 |
71104 |
> |
y(for)27 b(the)h(Lennard-Jones)e(and)i(dip)r(ole-dip)r(ole)g(in)n |
71105 |
> |
(teractions.)36 b(In)2042 4368 y(the)19 b(higher)g(temp)r(erature)f |
71106 |
> |
(sim)n(ulation)h(sho)n(wn)f(in)i(frames)e(C)h(and)2042 |
71107 |
> |
4464 y(D,)35 b(the)g(rep)r(eated)f(p)r(eak)g(features)g(are)g |
71108 |
> |
(signi\014can)n(tly)g(blurred.)2042 4559 y(The)21 b(\014rst)g(solv)-5 |
71109 |
> |
b(ation)20 b(shell)h(still)h(sho)n(ws)e(the)h(strong)f(e\013ect)i(of)f |
71110 |
> |
(the)2042 4655 y(stic)n(ky-p)r(oten)n(tial,)j(although)f(it)h(co)n(v)n |
71111 |
> |
(ers)e(a)i(larger)e(area,)h(extend-)2042 4750 y(ing)33 |
71112 |
> |
b(to)g(include)h(a)f(fraction)f(of)i(aligned)e(dip)r(ole)i(p)r(eaks)f |
71113 |
> |
(within)2042 4846 y(the)d(\014rst)g(solv)-5 b(ation)30 |
71114 |
> |
b(shell.)44 b(The)31 b(latter)f(p)r(eaks)f(lose)h(de\014nition)2042 |
71115 |
> |
4941 y(as)f(thermal)g(motion)g(and)h(the)g(comp)r(eting)g(dip)r(ole)f |
71116 |
> |
(force)g(o)n(v)n(er-)2042 5037 y(comes)23 b(the)h(stic)n(ky)g(p)r(oten) |
71117 |
> |
n(tial's)f(tigh)n(t)h(tetrahedral)f(structuring)2042 |
71118 |
> |
5132 y(of)k(the)h(\015uid.)2125 5228 y(This)k(complex)g(in)n(terpla)n |
71119 |
> |
(y)f(b)r(et)n(w)n(een)h(dip)r(ole)h(and)f(stic)n(ky)f(in-)2042 |
71120 |
> |
5323 y(teractions)37 b(w)n(as)g(remark)n(ed)f(up)r(on)i(as)f(a)h(p)r |
71121 |
> |
(ossible)f(reason)g(for)p eop |
71122 |
|
%%Page: 6 6 |
71123 |
< |
6 5 bop 4043 -299 a Fu(6)-150 -83 y(ice)36 b Fj(I)19 |
79495 |
< |
-71 y Fi(c)89 -83 y Fu(sim)n(ulation.)62 b(The)36 b(\014rst)g(p)r(eak)g |
79496 |
< |
(of)g(the)g(g\()p Fm(r)9 b Fu(\))36 b(primarily)-150 |
79497 |
< |
12 y(consists)23 b(of)h(the)g(preferred)f(h)n(ydrogen)f(b)r(onding)i |
79498 |
< |
(arrangemen)n(ts)-150 108 y(as)i(dictated)i(b)n(y)e(the)i(tetrahedral)e |
79499 |
< |
(stic)n(ky)g(p)r(oten)n(tial,)h(one)g(p)r(eak)-150 203 |
79500 |
< |
y(for)j(the)i(donating)e(and)h(the)g(other)g(for)f(the)i(accepting)e(h) |
79501 |
< |
n(ydro-)-150 299 y(gen)39 b(b)r(onds.)73 b(Due)40 b(to)g(the)g(high)g |
79502 |
< |
(degree)e(of)i(crystallinit)n(y)e(of)-150 394 y(the)e(sample,)i(the)f |
79503 |
< |
(second)e(and)h(third)g(solv)-5 b(ation)36 b(shells)f(sho)n(w)-150 |
79504 |
< |
490 y(a)30 b(rep)r(eated)h(p)r(eak)f(arrangemen)n(t)f(whic)n(h)i(deca)n |
79505 |
< |
(ys)e(at)i(distances)-150 585 y(around)20 b(the)h(fourth)g(solv)-5 |
79506 |
< |
b(ation)19 b(shell,)j(near)e(the)h(imp)r(osed)g(cuto\013)-150 |
79507 |
< |
681 y(for)27 b(the)i(Lennard-Jones)c(and)j(dip)r(ole-dip)r(ole)g(in)n |
79508 |
< |
(teractions.)36 b(In)-150 776 y(the)20 b(higher)e(temp)r(erature)h(sim) |
79509 |
< |
n(ulation)f(sho)n(wn)h(in)g(frames)f(C)i(and)-150 872 |
79510 |
< |
y(D,)35 b(the)g(rep)r(eated)f(p)r(eak)h(features)f(are)f(signi\014can)n |
79511 |
< |
(tly)h(blurred.)-150 967 y(The)21 b(\014rst)g(solv)-5 |
79512 |
< |
b(ation)20 b(shell)h(still)h(sho)n(ws)e(the)h(strong)f(e\013ect)i(of)f |
79513 |
< |
(the)-150 1063 y(stic)n(ky-p)r(oten)n(tial,)j(although)f(it)i(co)n(v)n |
79514 |
< |
(ers)c(a)j(larger)e(area,)i(extend-)-150 1158 y(ing)33 |
79515 |
< |
b(to)g(include)h(a)f(fraction)g(of)g(aligned)f(dip)r(ole)i(p)r(eaks)f |
79516 |
< |
(within)-150 1254 y(the)e(\014rst)f(solv)-5 b(ation)29 |
79517 |
< |
b(shell.)45 b(The)30 b(latter)g(p)r(eaks)g(lose)f(de\014nition)-150 |
79518 |
< |
1349 y(as)g(thermal)g(motion)h(and)f(the)h(comp)r(eting)g(dip)r(ole)g |
79519 |
< |
(force)f(o)n(v)n(er-)-150 1445 y(comes)23 b(the)i(stic)n(ky)e(p)r(oten) |
79520 |
< |
n(tial's)g(tigh)n(t)h(tetrahedral)f(structuring)-150 |
79521 |
< |
1540 y(of)28 b(the)g(\015uid.)-67 1636 y(This)k(complex)g(in)n(terpla)n |
79522 |
< |
(y)f(b)r(et)n(w)n(een)h(dip)r(ole)h(and)f(stic)n(ky)f(in-)-150 |
79523 |
< |
1731 y(teractions)37 b(w)n(as)g(remark)n(ed)f(up)r(on)i(as)f(a)h(p)r |
79524 |
< |
(ossible)g(reason)e(for)-150 1826 y(the)25 b(split)f(second)g(p)r(eak)g |
71123 |
> |
6 5 bop 4043 -299 a Fu(6)-150 -83 y(the)25 b(split)f(second)g(p)r(eak)g |
71124 |
|
(in)g(the)h(o)n(xygen-o)n(xygen)c(g\()p Fm(r)9 b Fu(\).)1592 |
71125 |
< |
1796 y Fn(5)1654 1826 y Fu(A)n(t)24 b(lo)n(w)-150 1922 |
71126 |
< |
y(temp)r(eratures,)h(the)h(second)f(solv)-5 b(ation)24 |
71127 |
< |
b(shell)h(p)r(eak)g(app)r(ears)g(to)-150 2017 y(ha)n(v)n(e)k(t)n(w)n(o) |
71128 |
< |
h(distinct)h(parts)f(that)g(blend)h(together)e(to)i(form)f(one)-150 |
71129 |
< |
2113 y(observ)-5 b(able)22 b(p)r(eak.)36 b(A)n(t)23 b(higher)g(temp)r |
71130 |
< |
(eratures,)h(this)g(split)g(c)n(har-)-150 2208 y(acter)k(alters)h(to)g |
71131 |
< |
(sho)n(w)f(the)i(leading)e(4)1101 2193 y(\027)1101 2208 |
71132 |
< |
y(A)i(p)r(eak)f(dominated)g(b)n(y)-150 2304 y(equatorial)i(an)n |
71133 |
< |
(ti-parallel)h(dip)r(ole)h(orien)n(tations,)g(and)g(there)g(is)-150 |
71134 |
< |
2399 y(tigh)n(tly)k(bunc)n(hed)h(group)f(of)g(axially)f(arranged)g(dip) |
71135 |
< |
r(oles)h(that)-150 2495 y(most)29 b(lik)n(ely)f(consist)h(of)f(the)i |
71136 |
< |
(smaller)e(fraction)g(aligned)g(dip)r(ole)-150 2590 y(pairs.)36 |
71137 |
< |
b(The)27 b(trailing)f(part)g(of)h(the)g(split)h(p)r(eak)e(at)h(5)1513 |
71138 |
< |
2575 y(\027)1513 2590 y(A)g(is)g(domi-)-150 2686 y(nated)f(b)n(y)g |
71139 |
< |
(aligned)g(dip)r(oles)g(that)g(range)f(primarily)g(within)i(the)-150 |
71140 |
< |
2781 y(axial)c(to)h(the)h(c)n(hief)f(h)n(ydrogen)e(b)r(ond)j |
71141 |
< |
(arrangemen)n(ts)c(similar)j(to)-150 2877 y(those)g(seen)g(in)h(the)f |
71142 |
< |
(\014rst)h(solv)-5 b(ation)23 b(shell.)36 b(This)24 b(evidence)g(indi-) |
71143 |
< |
-150 2972 y(cates)h(that)g(the)h(dip)r(ole)f(pair)g(in)n(teraction)f(b) |
71144 |
< |
r(egins)h(to)h(dominate)-150 3068 y(outside)31 b(of)g(the)g(range)f(of) |
71145 |
< |
h(the)g(dip)r(olar)g(repulsion)f(term,)i(with)-150 3163 |
71146 |
< |
y(the)e(primary)f(energetically)f(fa)n(v)n(orable)g(dip)r(ole)i |
71147 |
< |
(arrangemen)n(ts)-150 3259 y(p)r(opulating)j(the)h(region)e |
71148 |
< |
(immediately)i(outside)g(of)f(it's)h(range)-150 3354 |
71149 |
< |
y(\(around)24 b(4)228 3339 y(\027)228 3354 y(A\),)i(and)f(arrangemen)n |
71150 |
< |
(ts)e(that)j(seek)e(to)h(ideally)g(sat-)-150 3450 y(isfy)33 |
71151 |
< |
b(b)r(oth)g(the)g(stic)n(ky)f(and)g(dip)r(ole)h(forces)f(lo)r(cate)g |
71152 |
< |
(themselv)n(es)-150 3545 y(just)c(b)r(ey)n(ond)f(this)h(region)f |
71153 |
< |
(\(around)g(5)1097 3530 y(\027)1097 3545 y(A\).)-67 3641 |
71154 |
< |
y(F)-7 b(rom)25 b(these)h(\014ndings,)f(the)h(split)g(second)f(p)r(eak) |
71155 |
< |
g(is)g(primarily)-150 3736 y(the)35 b(pro)r(duct)g(of)f(the)i(dip)r |
71156 |
< |
(olar)e(repulsion)g(term)g(of)h(the)g(stic)n(ky)-150 |
71157 |
< |
3831 y(p)r(oten)n(tial.)56 b(In)34 b(fact,)h(the)g(leading)e(of)h(the)g |
71158 |
< |
(t)n(w)n(o)f(p)r(eaks)h(can)f(b)r(e)-150 3927 y(pushed)25 |
71159 |
< |
b(out)h(and)f(merged)f(with)i(the)g(outer)e(split)i(p)r(eak)f(just)h(b) |
71160 |
< |
n(y)-150 4022 y(extending)h(the)g(switc)n(hing)f(function)i(cuto\013)f |
71161 |
< |
(\()p Fj(s)1366 3992 y Ft(0)1389 4022 y Fu(\()p Fj(r)1458 |
71162 |
< |
4034 y Fi(ij)1517 4022 y Fu(\)\))h(from)e(its)-150 4127 |
71163 |
< |
y(normal)k(4.0)272 4112 y(\027)272 4127 y(A)h(to)g(v)-5 |
71164 |
< |
b(alues)31 b(of)g(4.5)f(or)g(ev)n(en)g(5)1326 4112 y(\027)1326 |
79566 |
< |
4127 y(A.)h(This)g(t)n(yp)r(e)g(of)-150 4222 y(correction)f(is)i(not)g |
71125 |
> |
-113 y Fn(5)1654 -83 y Fu(A)n(t)24 b(lo)n(w)-150 12 y(temp)r(eratures,) |
71126 |
> |
h(the)h(second)f(solv)-5 b(ation)24 b(shell)h(p)r(eak)g(app)r(ears)g |
71127 |
> |
(to)-150 108 y(ha)n(v)n(e)k(t)n(w)n(o)h(distinct)h(parts)f(that)g |
71128 |
> |
(blend)h(together)e(to)i(form)f(one)-150 203 y(observ)-5 |
71129 |
> |
b(able)22 b(p)r(eak.)36 b(A)n(t)23 b(higher)g(temp)r(eratures,)h(this)g |
71130 |
> |
(split)g(c)n(har-)-150 299 y(acter)k(alters)h(to)g(sho)n(w)f(the)i |
71131 |
> |
(leading)e(4)1101 284 y(\027)1101 299 y(A)i(p)r(eak)f(dominated)g(b)n |
71132 |
> |
(y)-150 394 y(equatorial)i(an)n(ti-parallel)h(dip)r(ole)h(orien)n |
71133 |
> |
(tations,)g(and)g(there)g(is)-150 490 y(tigh)n(tly)k(bunc)n(hed)h |
71134 |
> |
(group)f(of)g(axially)f(arranged)g(dip)r(oles)h(that)-150 |
71135 |
> |
585 y(most)29 b(lik)n(ely)f(consist)h(of)f(the)i(smaller)e(fraction)g |
71136 |
> |
(aligned)g(dip)r(ole)-150 681 y(pairs.)36 b(The)27 b(trailing)f(part)g |
71137 |
> |
(of)h(the)g(split)h(p)r(eak)e(at)h(5)1513 666 y(\027)1513 |
71138 |
> |
681 y(A)g(is)g(domi-)-150 776 y(nated)f(b)n(y)g(aligned)g(dip)r(oles)g |
71139 |
> |
(that)g(range)f(primarily)g(within)i(the)-150 872 y(axial)c(to)h(the)h |
71140 |
> |
(c)n(hief)f(h)n(ydrogen)e(b)r(ond)j(arrangemen)n(ts)c(similar)j(to)-150 |
71141 |
> |
967 y(those)g(seen)g(in)h(the)f(\014rst)h(solv)-5 b(ation)23 |
71142 |
> |
b(shell.)36 b(This)24 b(evidence)g(indi-)-150 1063 y(cates)h(that)g |
71143 |
> |
(the)h(dip)r(ole)f(pair)g(in)n(teraction)f(b)r(egins)h(to)h(dominate) |
71144 |
> |
-150 1158 y(outside)31 b(of)g(the)g(range)f(of)h(the)g(dip)r(olar)g |
71145 |
> |
(repulsion)f(term,)i(with)-150 1254 y(the)e(primary)f(energetically)f |
71146 |
> |
(fa)n(v)n(orable)g(dip)r(ole)i(arrangemen)n(ts)-150 1349 |
71147 |
> |
y(p)r(opulating)j(the)h(region)e(immediately)i(outside)g(of)f(it's)h |
71148 |
> |
(range)-150 1445 y(\(around)24 b(4)228 1430 y(\027)228 |
71149 |
> |
1445 y(A\),)i(and)f(arrangemen)n(ts)e(that)j(seek)e(to)h(ideally)g |
71150 |
> |
(sat-)-150 1540 y(isfy)33 b(b)r(oth)g(the)g(stic)n(ky)f(and)g(dip)r |
71151 |
> |
(ole)h(forces)f(lo)r(cate)g(themselv)n(es)-150 1636 y(just)c(b)r(ey)n |
71152 |
> |
(ond)f(this)h(region)f(\(around)g(5)1097 1621 y(\027)1097 |
71153 |
> |
1636 y(A\).)-67 1731 y(F)-7 b(rom)25 b(these)h(\014ndings,)f(the)h |
71154 |
> |
(split)g(second)f(p)r(eak)g(is)g(primarily)-150 1826 |
71155 |
> |
y(the)35 b(pro)r(duct)g(of)f(the)i(dip)r(olar)e(repulsion)g(term)g(of)h |
71156 |
> |
(the)g(stic)n(ky)-150 1922 y(p)r(oten)n(tial.)56 b(In)34 |
71157 |
> |
b(fact,)h(the)g(leading)e(of)h(the)g(t)n(w)n(o)f(p)r(eaks)h(can)f(b)r |
71158 |
> |
(e)-150 2017 y(pushed)25 b(out)h(and)f(merged)f(with)i(the)g(outer)e |
71159 |
> |
(split)i(p)r(eak)f(just)h(b)n(y)-150 2113 y(extending)h(the)g(switc)n |
71160 |
> |
(hing)f(function)i(cuto\013)f(\()p Fj(s)1366 2083 y Ft(0)1389 |
71161 |
> |
2113 y Fu(\()p Fj(r)1458 2125 y Fi(ij)1517 2113 y Fu(\)\))h(from)e(its) |
71162 |
> |
-150 2217 y(normal)k(4.0)272 2202 y(\027)272 2217 y(A)h(to)g(v)-5 |
71163 |
> |
b(alues)31 b(of)g(4.5)f(or)g(ev)n(en)g(5)1326 2202 y(\027)1326 |
71164 |
> |
2217 y(A.)h(This)g(t)n(yp)r(e)g(of)-150 2313 y(correction)f(is)i(not)g |
71165 |
|
(recommended)f(for)g(impro)n(ving)g(the)h(liquid)-150 |
71166 |
< |
4318 y(structure,)c(b)r(ecause)f(the)h(second)g(solv)-5 |
71167 |
< |
b(ation)27 b(shell)h(will)g(still)g(b)r(e)-150 4413 y(shifted)g(to)r(o) |
71166 |
> |
2408 y(structure,)c(b)r(ecause)f(the)h(second)g(solv)-5 |
71167 |
> |
b(ation)27 b(shell)h(will)g(still)g(b)r(e)-150 2504 y(shifted)g(to)r(o) |
71168 |
|
e(far)g(out.)37 b(In)27 b(addition,)g(this)g(w)n(ould)g(ha)n(v)n(e)e |
71169 |
< |
(an)i(ev)n(en)-150 4509 y(more)i(detrimen)n(tal)h(e\013ect)g(on)g(the)h |
71170 |
< |
(system)e(densities,)i(leading)-150 4604 y(to)40 b(a)g(liquid)h(with)f |
71169 |
> |
(an)i(ev)n(en)-150 2599 y(more)i(detrimen)n(tal)h(e\013ect)g(on)g(the)h |
71170 |
> |
(system)e(densities,)i(leading)-150 2695 y(to)40 b(a)g(liquid)h(with)f |
71171 |
|
(a)g(more)g(op)r(en)g(structure)g(and)g(a)g(densit)n(y)-150 |
71172 |
< |
4700 y(considerably)24 b(lo)n(w)n(er)f(than)i(the)h(normal)e(SSD)h(b)r |
71173 |
< |
(eha)n(vior)f(sho)n(wn)-150 4795 y(previously)-7 b(.)47 |
71172 |
> |
2790 y(considerably)24 b(lo)n(w)n(er)f(than)i(the)h(normal)e(SSD)h(b)r |
71173 |
> |
(eha)n(vior)f(sho)n(wn)-150 2886 y(previously)-7 b(.)47 |
71174 |
|
b(A)31 b(b)r(etter)h(correction)e(w)n(ould)h(b)r(e)g(to)g(include)h |
71175 |
< |
(the)-150 4891 y(quadrup)r(ole-quadrup)r(ole)e(in)n(teractions)h(for)h |
71176 |
< |
(the)g(w)n(ater)f(parti-)-150 4986 y(cles)h(outside)h(of)f(the)h |
71175 |
> |
(the)-150 2981 y(quadrup)r(ole-quadrup)r(ole)e(in)n(teractions)h(for)h |
71176 |
> |
(the)g(w)n(ater)f(parti-)-150 3077 y(cles)h(outside)h(of)f(the)h |
71177 |
|
(\014rst)g(solv)-5 b(ation)31 b(shell,)j(but)f(this)g(reduces)-150 |
71178 |
< |
5082 y(the)g(simplicit)n(y)f(and)h(sp)r(eed)g(adv)-5 |
71178 |
> |
3172 y(the)g(simplicit)n(y)f(and)h(sp)r(eed)g(adv)-5 |
71179 |
|
b(an)n(tage)30 b(of)j(SSD,)g(so)f(it)h(is)f(not)-150 |
71180 |
< |
5177 y(the)c(most)f(desirable)g(path)h(to)f(tak)n(e.)2070 |
71181 |
< |
-31 y Fr(T)-6 b(ABLE)26 b(I:)g(P)n(arameters)g(for)g(the)f(original)j |
71182 |
< |
(and)d(adjusted)h(mo)r(dels)p 2228 12 1644 4 v 2270 94 |
71183 |
< |
a(P)n(arameters)260 b(SSD)3054 63 y Fl(y)3222 94 y Fr(SSD/E)84 |
71184 |
< |
b(SSD/RF)p 2228 124 V 2322 205 a Fq(\033)28 b Fr(\()2424 |
71185 |
< |
192 y(\027)2424 205 y(A\))398 b(3.051)169 b(3.035)k(3.019)2322 |
71186 |
< |
292 y Fq(\017)25 b Fr(\(k)n(cal/mol\))178 b(0.152)169 |
71187 |
< |
b(0.152)k(0.152)2322 379 y Fq(\026)26 b Fr(\(D\))417 |
71188 |
< |
b(2.35)187 b(2.418)173 b(2.480)2322 467 y Fq(\027)2360 |
71189 |
< |
475 y Fc(0)2420 467 y Fr(\(k)n(cal/mol\))117 b(3.7284)169 |
71190 |
< |
b(3.90)211 b(3.90)2322 558 y Fq(r)2357 567 y Fp(l)2406 |
71191 |
< |
558 y Fr(\()2436 545 y(\027)2436 558 y(A\))406 b(2.75)206 |
71192 |
< |
b(2.40)211 b(2.40)2322 649 y Fq(r)2357 657 y Fp(u)2423 |
71193 |
< |
649 y Fr(\()2453 636 y(\027)2453 649 y(A\))389 b(3.35)206 |
71194 |
< |
b(3.80)211 b(3.80)2322 736 y Fq(\027)2365 705 y Fl(0)2360 |
71195 |
< |
749 y Fc(0)2420 736 y Fr(\(k)n(cal/mol\))117 b(3.7284)169 |
71196 |
< |
b(3.90)211 b(3.90)2322 828 y Fq(r)2359 796 y Fl(0)2357 |
71197 |
< |
843 y Fp(l)2406 828 y Fr(\()2436 815 y(\027)2436 828 |
71198 |
< |
y(A\))406 b(2.75)206 b(2.75)211 b(2.75)2322 919 y Fq(r)2359 |
71199 |
< |
887 y Fl(0)2357 932 y Fp(u)2423 919 y Fr(\()2453 906 |
71200 |
< |
y(\027)2453 919 y(A\))389 b(4.00)206 b(3.35)211 b(3.35)2245 |
71201 |
< |
1020 y Fl(y)2303 1051 y Fr(ref.)35 b(5)2158 1326 y Fo(D.)87 |
71202 |
< |
b(Adjusted)30 b(P)n(oten)n(tials:)40 b(SSD/E)29 b(and)h(SSD/RF)2125 |
71203 |
< |
1540 y Fu(The)i(prop)r(ensit)n(y)f(of)h(SSD)h(to)f(adopt)g(lo)n(w)n(er) |
71204 |
< |
f(than)h(exp)r(ected)2042 1636 y(densities)21 b(under)g(v)-5 |
71205 |
< |
b(arying)21 b(conditions)f(is)i(troubling,)g(esp)r(ecially)2042 |
71206 |
< |
1731 y(at)32 b(higher)f(temp)r(eratures.)50 b(In)32 b(order)f(to)h |
71207 |
< |
(correct)f(this)h(b)r(eha)n(v-)2042 1826 y(ior,)25 b(it's)h(necessary)d |
71208 |
< |
(to)j(adjust)g(the)f(force)g(\014eld)h(parameters)e(for)2042 |
71209 |
< |
1922 y(the)g(primary)e(in)n(termolecular)g(in)n(teractions.)35 |
71210 |
< |
b(In)23 b(undergoing)g(a)2042 2017 y(reparameterization,)30 |
71211 |
< |
b(it)j(is)f(imp)r(ortan)n(t)f(not)h(to)g(fo)r(cus)g(on)g(just)2042 |
71212 |
< |
2113 y(one)23 b(prop)r(ert)n(y)f(and)h(neglect)g(the)g(other)g(imp)r |
71213 |
< |
(ortan)n(t)g(prop)r(erties.)2042 2208 y(In)38 b(this)h(case,)h(it)f(w)n |
71214 |
< |
(ould)f(b)r(e)g(ideal)g(to)h(correct)d(the)j(densities)2042 |
71215 |
< |
2304 y(while)28 b(main)n(taining)e(the)i(accurate)f(transp)r(ort)f |
71216 |
< |
(prop)r(erties.)2125 2399 y(The)c(p)r(ossible)h(parameters)d(for)i |
71217 |
< |
(tuning)h(include)g(the)g Fj(\033)j Fu(and)c Fj(\017)2042 |
71218 |
< |
2495 y Fu(Lennard-Jones)28 b(parameters,)h(the)h(dip)r(ole)g(strength)g |
71219 |
< |
(\()p Fj(\026)p Fu(\),)h(and)2042 2590 y(the)20 b(stic)n(ky)f |
71220 |
< |
(attractiv)n(e)g(and)g(dip)r(ole)h(repulsiv)n(e)f(terms)g(with)h(their) |
71221 |
< |
2042 2686 y(resp)r(ectiv)n(e)31 b(cuto\013s.)51 b(T)-7 |
71222 |
< |
b(o)31 b(alter)h(the)g(attractiv)n(e)f(and)h(repulsiv)n(e)2042 |
71223 |
< |
2781 y(terms)h(of)g(the)h(stic)n(ky)f(p)r(oten)n(tial)g(indep)r(enden)n |
71224 |
< |
(tly)-7 b(,)36 b(it)e(is)f(neces-)2042 2877 y(sary)26 |
71225 |
< |
b(to)i(separate)e(the)i(terms)f(as)g(follo)n(ws:)2150 |
71226 |
< |
3076 y Fj(u)2198 3036 y Fi(sp)2198 3099 y(ij)2267 3076 |
71227 |
< |
y Fu(\()p Fh(r)2338 3088 y Fi(ij)2398 3076 y Fj(;)14 |
71228 |
< |
b Fh(\012)2503 3088 y Fi(i)2531 3076 y Fj(;)g Fh(\012)2637 |
71229 |
< |
3088 y Fi(j)2672 3076 y Fu(\))23 b(=)2825 3020 y Fj(\027)2866 |
71230 |
< |
3032 y Fn(0)p 2825 3057 79 4 v 2843 3133 a Fu(2)2913 |
71231 |
< |
3076 y([)p Fj(s)p Fu(\()p Fj(r)3044 3088 y Fi(ij)3103 |
71232 |
< |
3076 y Fu(\))p Fj(w)r Fu(\()p Fh(r)3267 3088 y Fi(ij)3327 |
71233 |
< |
3076 y Fj(;)14 b Fh(\012)3433 3088 y Fi(i)3461 3076 y |
71234 |
< |
Fj(;)g Fh(\012)3567 3088 y Fi(j)3602 3076 y Fu(\)])2833 |
71235 |
< |
3285 y(+)2926 3229 y Fj(\027)2972 3199 y Ft(0)2967 3249 |
71236 |
< |
y Fn(0)p 2926 3266 V 2945 3342 a Fu(2)3015 3285 y([)p |
71237 |
< |
Fj(s)3077 3251 y Ft(0)3100 3285 y Fu(\()p Fj(r)3169 3297 |
71238 |
< |
y Fi(ij)3228 3285 y Fu(\))p Fj(w)3321 3251 y Ft(0)3345 |
71239 |
< |
3285 y Fu(\()p Fh(r)3416 3297 y Fi(ij)3475 3285 y Fj(;)g |
71240 |
< |
Fh(\012)3581 3297 y Fi(i)3609 3285 y Fj(;)g Fh(\012)3715 |
71241 |
< |
3297 y Fi(j)3750 3285 y Fu(\)])p Fj(;)3937 3184 y Fu(\(10\))2125 |
71242 |
< |
3491 y(where)27 b Fj(\027)2406 3503 y Fn(0)2471 3491 |
71180 |
> |
3268 y(the)c(most)f(desirable)g(path)h(to)f(tak)n(e.)-34 |
71181 |
> |
3544 y Fo(D.)88 b(Adjusted)29 b(P)n(oten)n(tials:)40 |
71182 |
> |
b(SSD/E)30 b(and)f(SSD/RF)-67 3757 y Fu(The)j(prop)r(ensit)n(y)g(of)g |
71183 |
> |
(SSD)h(to)f(adopt)f(lo)n(w)n(er)g(than)h(exp)r(ected)-150 |
71184 |
> |
3853 y(densities)21 b(under)h(v)-5 b(arying)20 b(conditions)h(is)g |
71185 |
> |
(troubling,)h(esp)r(ecially)-150 3948 y(at)32 b(higher)f(temp)r |
71186 |
> |
(eratures.)50 b(In)32 b(order)f(to)h(correct)f(this)h(b)r(eha)n(v-)-150 |
71187 |
> |
4044 y(ior,)25 b(it's)h(necessary)e(to)h(adjust)h(the)g(force)e |
71188 |
> |
(\014eld)i(parameters)e(for)-150 4139 y(the)g(primary)e(in)n |
71189 |
> |
(termolecular)g(in)n(teractions.)35 b(In)24 b(undergoing)e(a)-150 |
71190 |
> |
4235 y(reparameterization,)31 b(it)h(is)g(imp)r(ortan)n(t)f(not)h(to)g |
71191 |
> |
(fo)r(cus)g(on)g(just)-150 4330 y(one)23 b(prop)r(ert)n(y)f(and)h |
71192 |
> |
(neglect)g(the)h(other)e(imp)r(ortan)n(t)h(prop)r(erties.)-150 |
71193 |
> |
4426 y(In)38 b(this)h(case,)h(it)f(w)n(ould)f(b)r(e)h(ideal)f(to)g |
71194 |
> |
(correct)f(the)h(densities)-150 4521 y(while)28 b(main)n(taining)f(the) |
71195 |
> |
h(accurate)e(transp)r(ort)h(prop)r(erties.)-67 4617 y(The)c(p)r |
71196 |
> |
(ossible)f(parameters)f(for)h(tuning)g(include)h(the)g |
71197 |
> |
Fj(\033)j Fu(and)d Fj(\017)-150 4712 y Fu(Lennard-Jones)28 |
71198 |
> |
b(parameters,)h(the)h(dip)r(ole)h(strength)e(\()p Fj(\026)p |
71199 |
> |
Fu(\),)j(and)-150 4807 y(the)20 b(stic)n(ky)f(attractiv)n(e)g(and)g |
71200 |
> |
(dip)r(ole)h(repulsiv)n(e)f(terms)g(with)h(their)-150 |
71201 |
> |
4903 y(resp)r(ectiv)n(e)31 b(cuto\013s.)51 b(T)-7 b(o)32 |
71202 |
> |
b(alter)f(the)i(attractiv)n(e)d(and)i(repulsiv)n(e)-150 |
71203 |
> |
4998 y(terms)h(of)g(the)h(stic)n(ky)f(p)r(oten)n(tial)g(indep)r(enden)n |
71204 |
> |
(tly)-7 b(,)36 b(it)e(is)f(neces-)2070 -31 y Fr(T)-6 |
71205 |
> |
b(ABLE)26 b(I:)g(P)n(arameters)g(for)g(the)f(original)j(and)d(adjusted) |
71206 |
> |
h(mo)r(dels)p 2228 12 1644 4 v 2270 94 a(P)n(arameters)260 |
71207 |
> |
b(SSD)3054 63 y Fl(y)3222 94 y Fr(SSD/E)84 b(SSD/RF)p |
71208 |
> |
2228 124 V 2322 205 a Fq(\033)28 b Fr(\()2424 192 y(\027)2424 |
71209 |
> |
205 y(A\))398 b(3.051)169 b(3.035)k(3.019)2322 292 y |
71210 |
> |
Fq(\017)25 b Fr(\(k)n(cal/mol\))178 b(0.152)169 b(0.152)k(0.152)2322 |
71211 |
> |
379 y Fq(\026)26 b Fr(\(D\))417 b(2.35)187 b(2.418)173 |
71212 |
> |
b(2.480)2322 467 y Fq(\027)2360 475 y Fc(0)2420 467 y |
71213 |
> |
Fr(\(k)n(cal/mol\))117 b(3.7284)169 b(3.90)211 b(3.90)2322 |
71214 |
> |
558 y Fq(r)2357 567 y Fp(l)2406 558 y Fr(\()2436 545 |
71215 |
> |
y(\027)2436 558 y(A\))406 b(2.75)206 b(2.40)211 b(2.40)2322 |
71216 |
> |
649 y Fq(r)2357 657 y Fp(u)2423 649 y Fr(\()2453 636 |
71217 |
> |
y(\027)2453 649 y(A\))389 b(3.35)206 b(3.80)211 b(3.80)2322 |
71218 |
> |
736 y Fq(\027)2365 705 y Fl(0)2360 749 y Fc(0)2420 736 |
71219 |
> |
y Fr(\(k)n(cal/mol\))117 b(3.7284)169 b(3.90)211 b(3.90)2322 |
71220 |
> |
828 y Fq(r)2359 796 y Fl(0)2357 843 y Fp(l)2406 828 y |
71221 |
> |
Fr(\()2436 815 y(\027)2436 828 y(A\))406 b(2.75)206 b(2.75)211 |
71222 |
> |
b(2.75)2322 919 y Fq(r)2359 887 y Fl(0)2357 932 y Fp(u)2423 |
71223 |
> |
919 y Fr(\()2453 906 y(\027)2453 919 y(A\))389 b(4.00)206 |
71224 |
> |
b(3.35)211 b(3.35)2245 1020 y Fl(y)2303 1051 y Fr(ref.)35 |
71225 |
> |
b(5)2042 1326 y Fu(sary)26 b(to)i(separate)e(the)i(terms)f(as)g(follo)n |
71226 |
> |
(ws:)2150 1526 y Fj(u)2198 1486 y Fi(sp)2198 1549 y(ij)2267 |
71227 |
> |
1526 y Fu(\()p Fh(r)2338 1538 y Fi(ij)2398 1526 y Fj(;)14 |
71228 |
> |
b Fh(\012)2503 1538 y Fi(i)2531 1526 y Fj(;)g Fh(\012)2637 |
71229 |
> |
1538 y Fi(j)2672 1526 y Fu(\))23 b(=)2825 1470 y Fj(\027)2866 |
71230 |
> |
1482 y Fn(0)p 2825 1507 79 4 v 2843 1583 a Fu(2)2913 |
71231 |
> |
1526 y([)p Fj(s)p Fu(\()p Fj(r)3044 1538 y Fi(ij)3103 |
71232 |
> |
1526 y Fu(\))p Fj(w)r Fu(\()p Fh(r)3267 1538 y Fi(ij)3327 |
71233 |
> |
1526 y Fj(;)14 b Fh(\012)3433 1538 y Fi(i)3461 1526 y |
71234 |
> |
Fj(;)g Fh(\012)3567 1538 y Fi(j)3602 1526 y Fu(\)])2833 |
71235 |
> |
1735 y(+)2926 1678 y Fj(\027)2972 1648 y Ft(0)2967 1699 |
71236 |
> |
y Fn(0)p 2926 1715 V 2945 1792 a Fu(2)3015 1735 y([)p |
71237 |
> |
Fj(s)3077 1700 y Ft(0)3100 1735 y Fu(\()p Fj(r)3169 1747 |
71238 |
> |
y Fi(ij)3228 1735 y Fu(\))p Fj(w)3321 1700 y Ft(0)3345 |
71239 |
> |
1735 y Fu(\()p Fh(r)3416 1747 y Fi(ij)3475 1735 y Fj(;)g |
71240 |
> |
Fh(\012)3581 1747 y Fi(i)3609 1735 y Fj(;)g Fh(\012)3715 |
71241 |
> |
1747 y Fi(j)3750 1735 y Fu(\)])p Fj(;)3937 1634 y Fu(\(10\))2125 |
71242 |
> |
1941 y(where)27 b Fj(\027)2406 1953 y Fn(0)2471 1941 |
71243 |
|
y Fu(scales)f(the)i(strength)f(of)g(the)h(tetrahedral)e(attrac-)2042 |
71244 |
< |
3586 y(tion)40 b(and)g Fj(\027)2445 3556 y Ft(0)2440 |
71245 |
< |
3607 y Fn(0)2517 3586 y Fu(acts)g(in)g(an)g(iden)n(tical)g(fashion)g |
71246 |
< |
(on)g(the)g(dip)r(ole)2042 3682 y(repulsion)29 b(term.)43 |
71244 |
> |
2036 y(tion)40 b(and)g Fj(\027)2445 2006 y Ft(0)2440 |
71245 |
> |
2057 y Fn(0)2517 2036 y Fu(acts)g(in)g(an)g(iden)n(tical)g(fashion)g |
71246 |
> |
(on)g(the)g(dip)r(ole)2042 2131 y(repulsion)29 b(term.)43 |
71247 |
|
b(F)-7 b(or)30 b(purp)r(oses)f(of)h(the)g(reparameterization,)2042 |
71248 |
< |
3777 y(the)j(separation)e(w)n(as)g(p)r(erformed,)i(but)h(the)f(\014nal) |
71249 |
< |
f(parameters)2042 3873 y(w)n(ere)h(adjusted)i(so)f(that)h(it)g(is)f |
71250 |
< |
(unnecessary)f(to)i(separate)e(the)2042 3968 y(terms)25 |
71248 |
> |
2227 y(the)j(separation)e(w)n(as)g(p)r(erformed,)i(but)h(the)f(\014nal) |
71249 |
> |
f(parameters)2042 2322 y(w)n(ere)h(adjusted)i(so)f(that)h(it)g(is)f |
71250 |
> |
(unnecessary)f(to)i(separate)e(the)2042 2418 y(terms)25 |
71251 |
|
b(when)i(implemen)n(ting)f(the)g(adjusted)h(w)n(ater)d(p)r(oten)n |
71252 |
< |
(tials.)2042 4064 y(The)e(results)g(of)h(the)g(reparameterizations)c |
71253 |
< |
(are)j(sho)n(wn)f(in)i(table)2042 4159 y(I.)60 b(Note)35 |
71254 |
< |
b(that)h(b)r(oth)f(the)h(tetrahedral)e(attractiv)n(e)g(and)h(dip)r(o-) |
71255 |
< |
2042 4255 y(lar)k(repulsiv)n(e)g(don't)h(share)f(the)h(same)g(lo)n(w)n |
71256 |
< |
(er)e(cuto\013)i(\()p Fj(r)3916 4267 y Fi(l)3943 4255 |
71257 |
< |
y Fu(\))g(in)2042 4350 y(the)d(newly)g(parameterized)f(p)r(oten)n |
71258 |
< |
(tials)h(-)f(soft)i(stic)n(ky)e(dip)r(ole)2042 4446 y(enhanced)f |
71252 |
> |
(tials.)2042 2513 y(The)e(results)g(of)h(the)g(reparameterizations)c |
71253 |
> |
(are)j(sho)n(wn)f(in)i(table)2042 2609 y(I.)60 b(Note)35 |
71254 |
> |
b(that)h(b)r(oth)f(the)h(tetrahedral)e(attractiv)n(e)g(and)h(dip)r(o-) |
71255 |
> |
2042 2704 y(lar)k(repulsiv)n(e)g(don't)h(share)f(the)h(same)g(lo)n(w)n |
71256 |
> |
(er)e(cuto\013)i(\()p Fj(r)3916 2716 y Fi(l)3943 2704 |
71257 |
> |
y Fu(\))g(in)2042 2800 y(the)d(newly)g(parameterized)f(p)r(oten)n |
71258 |
> |
(tials)h(-)f(soft)i(stic)n(ky)e(dip)r(ole)2042 2895 y(enhanced)f |
71259 |
|
(\(SSD/E\))h(and)f(soft)h(stic)n(ky)f(dip)r(ole)g(reaction)g(\014eld) |
71260 |
< |
2042 4541 y(\(SSD/RF\).)2125 4636 y(In)20 b(the)g(pap)r(er)f(detailing) |
71260 |
> |
2042 2991 y(\(SSD/RF\).)2125 3086 y(In)20 b(the)g(pap)r(er)f(detailing) |
71261 |
|
h(the)g(dev)n(elopmen)n(t)f(of)h(SSD,)g(Liu)g(and)2042 |
71262 |
< |
4732 y(Ic)n(hiy)n(e)h(placed)g(particular)g(emphasis)g(on)h(an)f |
71263 |
< |
(accurate)g(descrip-)2042 4827 y(tion)29 b(of)f(the)i(\014rst)e(solv)-5 |
71262 |
> |
3182 y(Ic)n(hiy)n(e)h(placed)g(particular)g(emphasis)g(on)h(an)f |
71263 |
> |
(accurate)g(descrip-)2042 3277 y(tion)29 b(of)f(the)i(\014rst)e(solv)-5 |
71264 |
|
b(ation)28 b(shell.)40 b(This)29 b(resulted)g(in)g(a)f(some-)2042 |
71265 |
< |
4923 y(what)40 b(tall)f(and)h(sharp)f(\014rst)h(p)r(eak)f(that)i(in)n |
71266 |
< |
(tegrated)d(to)i(giv)n(e)2042 5018 y(similar)35 b(co)r(ordination)g(n)n |
71265 |
> |
3373 y(what)40 b(tall)f(and)h(sharp)f(\014rst)h(p)r(eak)f(that)i(in)n |
71266 |
> |
(tegrated)d(to)i(giv)n(e)2042 3468 y(similar)35 b(co)r(ordination)g(n)n |
71267 |
|
(um)n(b)r(ers)g(to)h(the)g(exp)r(erimen)n(tal)g(data)2042 |
71268 |
< |
5114 y(obtained)26 b(b)n(y)g(Sop)r(er)f(and)h(Phillips.)3184 |
71269 |
< |
5084 y Fn(5,25)3333 5114 y Fu(New)g(exp)r(erimen)n(tal)g(x-)2042 |
71270 |
< |
5209 y(ra)n(y)i(scattering)h(data)g(from)h(the)g(Head-Gordon)e(lab)h |
71271 |
< |
(indicates)2042 5305 y(a)j(sligh)n(tly)f(lo)n(w)n(er)g(and)h(shifted)h |
71272 |
< |
(\014rst)f(p)r(eak)f(in)i(the)f(g)3743 5317 y Fn(OO)3849 |
71273 |
< |
5305 y Fu(\()p Fj(r)r Fu(\),)j(so)2042 5400 y(adjustmen)n(ts)25 |
71268 |
> |
3564 y(obtained)26 b(b)n(y)g(Sop)r(er)f(and)h(Phillips.)3184 |
71269 |
> |
3533 y Fn(5,25)3333 3564 y Fu(New)g(exp)r(erimen)n(tal)g(x-)2042 |
71270 |
> |
3659 y(ra)n(y)i(scattering)h(data)g(from)h(the)g(Head-Gordon)e(lab)h |
71271 |
> |
(indicates)2042 3755 y(a)j(sligh)n(tly)f(lo)n(w)n(er)g(and)h(shifted)h |
71272 |
> |
(\014rst)f(p)r(eak)f(in)i(the)f(g)3743 3767 y Fn(OO)3849 |
71273 |
> |
3755 y Fu(\()p Fj(r)r Fu(\),)j(so)2042 3850 y(adjustmen)n(ts)25 |
71274 |
|
b(to)h(SSD)g(w)n(ere)e(made)h(while)h(taking)f(in)n(to)g(consid-)2042 |
71275 |
< |
5496 y(eration)i(the)i(new)g(exp)r(erimen)n(tal)f(\014ndings.)3442 |
71276 |
< |
5466 y Fn(24)3540 5496 y Fu(Figure)g(7)g(sho)n(ws)p eop |
71275 |
> |
3945 y(eration)i(the)i(new)g(exp)r(erimen)n(tal)f(\014ndings.)3442 |
71276 |
> |
3915 y Fn(24)3540 3945 y Fu(Figure)g(6)g(sho)n(ws)2042 |
71277 |
> |
4041 y(the)23 b(relo)r(cation)f(of)i(the)f(\014rst)g(p)r(eak)g(of)h |
71278 |
> |
(the)f(o)n(xygen-o)n(xygen)d(g\()p Fm(r)9 b Fu(\))2042 |
71279 |
> |
4136 y(b)n(y)30 b(comparing)g(the)h(original)f(SSD)i(\(with)f(and)g |
71280 |
> |
(without)h(reac-)2042 4232 y(tion)24 b(\014eld\),)i(SSD-E,)e(and)g |
71281 |
> |
(SSD-RF)h(to)g(the)f(new)h(exp)r(erimen)n(tal)2042 4327 |
71282 |
> |
y(results.)71 b(Both)39 b(the)g(mo)r(di\014ed)h(w)n(ater)e(mo)r(dels)h |
71283 |
> |
(ha)n(v)n(e)f(shorter)2042 4423 y(p)r(eaks)23 b(that)h(are)f(brough)n |
71284 |
> |
(t)f(in)i(more)f(closely)g(to)h(the)g(exp)r(erimen-)2042 |
71285 |
> |
4518 y(tal)33 b(p)r(eak)g(\(as)h(seen)f(in)h(the)f(insets)h(of)f |
71286 |
> |
(\014gure)g(6\).)54 b(This)34 b(struc-)2042 4614 y(tural)c(alteration)g |
71287 |
> |
(w)n(as)g(accomplished)h(b)n(y)f(a)h(reduction)g(in)g(the)2042 |
71288 |
> |
4709 y(Lennard-Jones)k Fj(\033)41 b Fu(v)-5 b(ariable)37 |
71289 |
> |
b(as)g(w)n(ell)g(as)g(adjustmen)n(t)h(of)g(the)2042 4805 |
71290 |
> |
y(stic)n(ky)25 b(p)r(oten)n(tial)h(strength)f(and)h(cuto\013s.)37 |
71291 |
> |
b(The)25 b(cuto\013s)h(for)g(the)2042 4900 y(tetrahedral)34 |
71292 |
> |
b(attractiv)n(e)g(and)i(dip)r(olar)e(repulsiv)n(e)h(terms)g(w)n(ere) |
71293 |
> |
2042 4996 y(nearly)24 b(sw)n(app)r(ed)h(with)h(eac)n(h)f(other.)36 |
71294 |
> |
b(Isosurfaces)23 b(of)j(the)g(origi-)2042 5091 y(nal)h(and)g(mo)r |
71295 |
> |
(di\014ed)h(stic)n(ky)f(p)r(oten)n(tials)h(are)e(sho)n(wn)h(in)h |
71296 |
> |
(\014gure)3993 5061 y Fb(?)4061 5091 y Fu(.)2042 5187 |
71297 |
> |
y(In)22 b(these)h(isosurfaces,)f(it)h(is)f(easy)f(to)i(see)f(ho)n(w)g |
71298 |
> |
(altering)f(the)i(cut-)2042 5282 y(o\013s)i(c)n(hanges)f(the)i |
71299 |
> |
(repulsiv)n(e)e(and)i(attractiv)n(e)e(c)n(haracter)f(of)j(the)2042 |
71300 |
> |
5378 y(particles.)53 b(With)34 b(a)f(reduced)g(repulsiv)n(e)g(surface)f |
71301 |
> |
(\(the)i(dark)n(er)p eop |
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|
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7 6 bop 4043 -299 a Fu(7)-133 2930 y @beginspecial 71 |
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@llx 60 @lly 514 @urx 743 @ury 2409 @rwi @setspecial |
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@endspecial -150 3100 a Fr(FIG.)26 b(7:)34 b(Plots)27 |
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> |
@endspecial -150 3100 a Fr(FIG.)26 b(6:)34 b(Plots)27 |
86249 |
|
b(comparing)e(exp)r(erimen)n(t)1076 3068 y Fc(24)1165 |
86250 |
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3100 y Fr(with)g(SSD/E)g(and)g(SSD)-150 3187 y(without)c(reaction)g |
86251 |
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(\014eld)g(\(top\),)g(as)h(w)n(ell)f(as)h(SSD/RF)d(and)h(SSD)g(with) |
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< |
@endspecial -150 4970 a(FIG.)h(8:)36 b(Isosurfaces)29 |
480292 |
> |
@endspecial -150 4970 a(FIG.)h(7:)36 b(Isosurfaces)29 |
480293 |
|
b(of)e(the)f(stic)n(ky)g(p)r(oten)n(tial)h(for)g(SSD)f(\(left\))h(and) |
480294 |
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-150 5057 y(SSD/E)37 b(&)f(SSD/RF)h(\(righ)n(t\).)68 |
480295 |
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b(Ligh)n(t)37 b(areas)i(corresp)r(ond)e(to)h(the)-150 |
480296 |
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5144 y(tetrahedral)29 b(attractiv)n(e)h(part,)g(and)e(the)h(dark)n(er)g |
480297 |
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(areas)h(corresp)r(ond)-150 5231 y(to)c(the)f(dip)r(olar)i(repulsiv)n |
480298 |
< |
(e)e(part.)2042 -83 y Fu(the)e(relo)r(cation)f(of)i(the)f(\014rst)g(p)r |
480299 |
< |
(eak)g(of)h(the)f(o)n(xygen-o)n(xygen)d(g\()p Fm(r)9 |
480300 |
< |
b Fu(\))2042 12 y(b)n(y)30 b(comparing)g(the)h(original)f(SSD)i(\(with) |
480301 |
< |
f(and)g(without)h(reac-)2042 108 y(tion)24 b(\014eld\),)i(SSD-E,)e(and) |
480302 |
< |
g(SSD-RF)h(to)g(the)f(new)h(exp)r(erimen)n(tal)2042 203 |
480303 |
< |
y(results.)71 b(Both)39 b(the)g(mo)r(di\014ed)h(w)n(ater)e(mo)r(dels)h |
480304 |
< |
(ha)n(v)n(e)f(shorter)2042 299 y(p)r(eaks)23 b(that)h(are)f(brough)n(t) |
480305 |
< |
f(in)i(more)f(closely)g(to)h(the)g(exp)r(erimen-)2042 |
488683 |
< |
394 y(tal)33 b(p)r(eak)g(\(as)h(seen)f(in)h(the)f(insets)h(of)f |
488684 |
< |
(\014gure)g(7\).)54 b(This)34 b(struc-)2042 490 y(tural)c(alteration)g |
488685 |
< |
(w)n(as)g(accomplished)h(b)n(y)f(a)h(reduction)g(in)g(the)2042 |
488686 |
< |
585 y(Lennard-Jones)k Fj(\033)41 b Fu(v)-5 b(ariable)37 |
488687 |
< |
b(as)g(w)n(ell)g(as)g(adjustmen)n(t)h(of)g(the)2042 681 |
488688 |
< |
y(stic)n(ky)25 b(p)r(oten)n(tial)h(strength)f(and)h(cuto\013s.)37 |
488689 |
< |
b(The)25 b(cuto\013s)h(for)g(the)2042 776 y(tetrahedral)34 |
488690 |
< |
b(attractiv)n(e)g(and)i(dip)r(olar)e(repulsiv)n(e)h(terms)g(w)n(ere) |
488691 |
< |
2042 872 y(nearly)24 b(sw)n(app)r(ed)h(with)h(eac)n(h)f(other.)36 |
488692 |
< |
b(Isosurfaces)23 b(of)j(the)g(origi-)2042 967 y(nal)h(and)g(mo)r |
488693 |
< |
(di\014ed)h(stic)n(ky)f(p)r(oten)n(tials)h(are)e(sho)n(wn)h(in)h |
488694 |
< |
(\014gure)3993 937 y Fb(?)4061 967 y Fu(.)2042 1063 y(In)22 |
488695 |
< |
b(these)h(isosurfaces,)f(it)h(is)f(easy)f(to)i(see)f(ho)n(w)g(altering) |
488696 |
< |
f(the)i(cut-)2042 1158 y(o\013s)i(c)n(hanges)f(the)i(repulsiv)n(e)e |
488697 |
< |
(and)i(attractiv)n(e)e(c)n(haracter)f(of)j(the)2042 1254 |
488698 |
< |
y(particles.)53 b(With)34 b(a)f(reduced)g(repulsiv)n(e)g(surface)f |
488699 |
< |
(\(the)i(dark)n(er)2042 1349 y(region\),)25 b(the)h(particles)g(can)f |
488700 |
< |
(mo)n(v)n(e)g(closer)g(to)g(one)h(another,)f(in-)2042 |
488701 |
< |
1445 y(creasing)i(the)j(densit)n(y)e(for)h(the)g(o)n(v)n(erall)e |
488702 |
< |
(system.)41 b(This)29 b(c)n(hange)2042 1540 y(in)d(in)n(teraction)e |
488703 |
< |
(cuto\013)i(also)f(results)g(in)h(a)f(more)g(gradual)f(orien-)2042 |
488704 |
< |
1636 y(tational)c(motion)g(b)n(y)g(allo)n(wing)f(the)i(particles)f(to)g |
488705 |
< |
(main)n(tain)g(pre-)2042 1731 y(ferred)k(dip)r(olar)g(arrangemen)n(ts)f |
488706 |
< |
(b)r(efore)i(they)g(b)r(egin)g(to)g(feel)g(the)2042 1826 |
480298 |
> |
(e)e(part.)2042 -83 y Fu(region\),)g(the)h(particles)g(can)f(mo)n(v)n |
480299 |
> |
(e)g(closer)g(to)g(one)h(another,)f(in-)2042 12 y(creasing)i(the)j |
480300 |
> |
(densit)n(y)e(for)h(the)g(o)n(v)n(erall)e(system.)41 |
480301 |
> |
b(This)29 b(c)n(hange)2042 108 y(in)d(in)n(teraction)e(cuto\013)i(also) |
480302 |
> |
f(results)g(in)h(a)f(more)g(gradual)f(orien-)2042 203 |
480303 |
> |
y(tational)c(motion)g(b)n(y)g(allo)n(wing)f(the)i(particles)f(to)g |
480304 |
> |
(main)n(tain)g(pre-)2042 299 y(ferred)k(dip)r(olar)g(arrangemen)n(ts)f |
480305 |
> |
(b)r(efore)i(they)g(b)r(egin)g(to)g(feel)g(the)2042 394 |
480306 |
|
y(pull)c(of)g(the)g(tetrahedral)f(restructuring.)33 b(Up)r(on)22 |
480307 |
< |
b(mo)n(ving)d(closer)2042 1922 y(together,)28 b(the)h(dip)r(olar)e |
480307 |
> |
b(mo)n(ving)d(closer)2042 490 y(together,)28 b(the)h(dip)r(olar)e |
480308 |
|
(repulsion)h(term)g(b)r(ecomes)h(activ)n(e)e(and)2042 |
480309 |
< |
2017 y(excludes)39 b(the)h(unph)n(ysical)f(arrangemen)n(ts.)70 |
480310 |
< |
b(This)40 b(compares)2042 2113 y(with)25 b(the)g(original)e(SSD's)i |
480309 |
> |
585 y(excludes)39 b(the)h(unph)n(ysical)f(arrangemen)n(ts.)70 |
480310 |
> |
b(This)40 b(compares)2042 681 y(with)25 b(the)g(original)e(SSD's)i |
480311 |
|
(excluding)f(dip)r(olar)g(b)r(efore)g(the)h(par-)2042 |
480312 |
< |
2208 y(ticles)k(feel)h(the)f(pull)h(of)f(the)h(\\h)n(ydrogen)d(b)r |
480313 |
< |
(onds".)41 b(Aside)30 b(from)2042 2304 y(impro)n(ving)35 |
480312 |
> |
776 y(ticles)k(feel)h(the)f(pull)h(of)f(the)h(\\h)n(ydrogen)d(b)r |
480313 |
> |
(onds".)41 b(Aside)30 b(from)2042 872 y(impro)n(ving)35 |
480314 |
|
b(the)i(shap)r(e)f(of)h(the)g(\014rst)f(p)r(eak)g(in)h(the)g(g\()p |
480315 |
< |
Fm(r)9 b Fu(\),)39 b(this)2042 2399 y(impro)n(v)n(es)27 |
480315 |
> |
Fm(r)9 b Fu(\),)39 b(this)2042 967 y(impro)n(v)n(es)27 |
480316 |
|
b(the)h(densities)h(considerably)e(b)n(y)h(allo)n(wing)f(the)i(p)r(er-) |
480317 |
< |
2042 2495 y(sistence)j(of)g(full)g(dip)r(olar)g(c)n(haracter)e(b)r(elo) |
480318 |
< |
n(w)i(the)g(previous)f(4.0)2042 2575 y(\027)2042 2590 |
480319 |
< |
y(A)d(cuto\013.)2125 2686 y(While)43 b(adjusting)f(the)h(lo)r(cation)f |
480320 |
< |
(and)h(shap)r(e)f(of)h(the)f(\014rst)2042 2781 y(p)r(eak)23 |
480317 |
> |
2042 1063 y(sistence)j(of)g(full)g(dip)r(olar)g(c)n(haracter)e(b)r(elo) |
480318 |
> |
n(w)i(the)g(previous)f(4.0)2042 1143 y(\027)2042 1158 |
480319 |
> |
y(A)d(cuto\013.)2125 1254 y(While)43 b(adjusting)f(the)h(lo)r(cation)f |
480320 |
> |
(and)h(shap)r(e)f(of)h(the)f(\014rst)2042 1349 y(p)r(eak)23 |
480321 |
|
b(of)h(g\()p Fm(r)9 b Fu(\))24 b(impro)n(v)n(es)e(the)i(densities)g(to) |
480322 |
< |
f(some)h(degree,)f(these)2042 2877 y(c)n(hanges)34 b(alone)i(are)f |
480322 |
> |
f(some)h(degree,)f(these)2042 1445 y(c)n(hanges)34 b(alone)i(are)f |
480323 |
|
(insu\016cien)n(t)h(to)g(bring)g(the)g(system)g(den-)2042 |
480324 |
< |
2972 y(sities)c(up)h(to)g(the)g(v)-5 b(alues)32 b(observ)n(ed)f(exp)r |
480324 |
> |
1540 y(sities)c(up)h(to)g(the)g(v)-5 b(alues)32 b(observ)n(ed)f(exp)r |
480325 |
|
(erimen)n(tally)-7 b(.)51 b(T)-7 b(o)32 b(\014n-)2042 |
480326 |
< |
3068 y(ish)i(bringing)f(up)i(the)f(densities,)i(the)f(dip)r(ole)f |
480327 |
< |
(momen)n(ts)g(w)n(ere)2042 3163 y(increased)g(in)h(b)r(oth)h(the)g |
480326 |
> |
1636 y(ish)i(bringing)f(up)i(the)f(densities,)i(the)f(dip)r(ole)f |
480327 |
> |
(momen)n(ts)g(w)n(ere)2042 1731 y(increased)g(in)h(b)r(oth)h(the)g |
480328 |
|
(adjusted)f(mo)r(dels.)60 b(Being)35 b(a)g(dip)r(ole)2042 |
480329 |
< |
3259 y(based)e(mo)r(del,)i(the)f(structure)f(and)g(transp)r(ort)g(are)f |
480330 |
< |
(v)n(ery)h(sen-)2042 3354 y(sitiv)n(e)40 b(to)h(c)n(hanges)f(in)h(the)h |
480331 |
< |
(dip)r(ole)f(momen)n(t.)77 b(The)41 b(original)2042 3450 |
480332 |
< |
y(SSD)27 b(simply)f(used)h(the)f(dip)r(ole)h(momen)n(t)f(calculated)g |
480333 |
< |
(from)g(the)2042 3545 y(TIP3P)44 b(w)n(ater)h(mo)r(del,)50 |
480329 |
> |
1826 y(based)e(mo)r(del,)i(the)f(structure)f(and)g(transp)r(ort)g(are)f |
480330 |
> |
(v)n(ery)h(sen-)2042 1922 y(sitiv)n(e)40 b(to)h(c)n(hanges)f(in)h(the)h |
480331 |
> |
(dip)r(ole)f(momen)n(t.)77 b(The)41 b(original)2042 2017 |
480332 |
> |
y(SSD)27 b(simply)f(used)h(the)f(dip)r(ole)h(momen)n(t)f(calculated)g |
480333 |
> |
(from)g(the)2042 2113 y(TIP3P)44 b(w)n(ater)h(mo)r(del,)50 |
480334 |
|
b(whic)n(h)c(at)f(2.35)f(D)j(is)e(signi\014can)n(tly)2042 |
480335 |
< |
3641 y(greater)24 b(than)h(the)h(exp)r(erimen)n(tal)g(gas)e(phase)h(v) |
480336 |
< |
-5 b(alue)26 b(of)f(1.84)g(D.)2042 3736 y(The)33 b(larger)e(dip)r(ole)j |
480335 |
> |
2208 y(greater)24 b(than)h(the)h(exp)r(erimen)n(tal)g(gas)e(phase)h(v) |
480336 |
> |
-5 b(alue)26 b(of)f(1.84)g(D.)2042 2304 y(The)33 b(larger)e(dip)r(ole)j |
480337 |
|
(momen)n(t)f(is)g(a)g(more)f(realistic)g(v)-5 b(alue)33 |
480338 |
< |
b(and)2042 3831 y(impro)n(v)n(e)24 b(the)i(dielectric)g(prop)r(erties)f |
480339 |
< |
(of)h(the)g(\015uid.)37 b(Both)26 b(theo-)2042 3927 y(retical)h(and)i |
480338 |
> |
b(and)2042 2399 y(impro)n(v)n(e)24 b(the)i(dielectric)g(prop)r(erties)f |
480339 |
> |
(of)h(the)g(\015uid.)37 b(Both)26 b(theo-)2042 2495 y(retical)h(and)i |
480340 |
|
(exp)r(erimen)n(tal)e(measuremen)n(ts)h(indicate)g(a)g(liquid)2042 |
480341 |
< |
4022 y(phase)18 b(dip)r(ole)i(momen)n(t)f(ranging)e(from)i(2.4)f(D)i |
480342 |
< |
(to)f(v)-5 b(alues)19 b(as)f(high)2042 4118 y(as)29 b(3.11)g(D,)i(so)e |
480341 |
> |
2590 y(phase)18 b(dip)r(ole)i(momen)n(t)f(ranging)e(from)i(2.4)f(D)i |
480342 |
> |
(to)f(v)-5 b(alues)19 b(as)f(high)2042 2686 y(as)29 b(3.11)g(D,)i(so)e |
480343 |
|
(there)h(is)g(quite)g(a)g(range)f(a)n(v)-5 b(ailable)29 |
480344 |
< |
b(for)g(adjust-)2042 4213 y(ing)c(the)i(dip)r(ole)e(momen)n(t.)2880 |
480345 |
< |
4183 y Fn(26)q({29)3076 4213 y Fu(The)h(increasing)e(of)i(the)g(dip)r |
480346 |
< |
(ole)2042 4309 y(momen)n(ts)34 b(to)g(2.418)f(and)h(2.48)f(D)i(for)e |
480347 |
< |
(SSD/E)h(and)h(SSD/RF)2042 4404 y(resp)r(ectiv)n(ely)c(is)g(mo)r |
480344 |
> |
b(for)g(adjust-)2042 2781 y(ing)c(the)i(dip)r(ole)e(momen)n(t.)2880 |
480345 |
> |
2751 y Fn(26)q({29)3076 2781 y Fu(The)h(increasing)e(of)i(the)g(dip)r |
480346 |
> |
(ole)2042 2877 y(momen)n(ts)34 b(to)g(2.418)f(and)h(2.48)f(D)i(for)e |
480347 |
> |
(SSD/E)h(and)h(SSD/RF)2042 2972 y(resp)r(ectiv)n(ely)c(is)g(mo)r |
480348 |
|
(derate)h(in)g(the)g(range)f(of)g(the)i(exp)r(erimen-)2042 |
480349 |
< |
4500 y(tal)27 b(v)-5 b(alues;)27 b(ho)n(w)n(ev)n(er,)f(it)i(leads)f(to) |
480350 |
< |
g(signi\014can)n(t)g(c)n(hanges)f(in)i(the)2042 4595 |
480349 |
> |
3068 y(tal)27 b(v)-5 b(alues;)27 b(ho)n(w)n(ev)n(er,)f(it)i(leads)f(to) |
480350 |
> |
g(signi\014can)n(t)g(c)n(hanges)f(in)i(the)2042 3163 |
480351 |
|
y(densit)n(y)f(and)h(transp)r(ort)e(of)i(the)g(w)n(ater)e(mo)r(dels.) |
480352 |
< |
2125 4691 y(In)31 b(order)e(to)i(demonstrate)f(the)i(b)r(ene\014ts)f |
480353 |
< |
(of)g(this)g(reparam-)2042 4786 y(eterization,)i(a)g(series)f(of)h(NPT) |
480354 |
< |
g(and)g(NVE)g(sim)n(ulations)f(w)n(ere)2042 4882 y(p)r(erformed)25 |
480352 |
> |
2125 3259 y(In)31 b(order)e(to)i(demonstrate)f(the)i(b)r(ene\014ts)f |
480353 |
> |
(of)g(this)g(reparam-)2042 3354 y(eterization,)i(a)g(series)f(of)h(NPT) |
480354 |
> |
g(and)g(NVE)g(sim)n(ulations)f(w)n(ere)2042 3450 y(p)r(erformed)25 |
480355 |
|
b(to)h(prob)r(e)g(the)g(densit)n(y)g(and)g(transp)r(ort)f(prop)r |
480356 |
< |
(erties)2042 4977 y(of)37 b(the)h(adapted)f(mo)r(dels)h(and)f(compare)f |
480357 |
< |
(the)i(results)f(to)h(the)2042 5073 y(original)26 b(SSD)j(mo)r(del.)37 |
480356 |
> |
(erties)2042 3545 y(of)37 b(the)h(adapted)f(mo)r(dels)h(and)f(compare)f |
480357 |
> |
(the)i(results)f(to)h(the)2042 3641 y(original)26 b(SSD)j(mo)r(del.)37 |
480358 |
|
b(This)28 b(comparison)e(in)n(v)n(olv)n(ed)h(full)h(NPT)2042 |
480359 |
< |
5168 y(melting)f(sequences)f(for)g(b)r(oth)i(SSD/E)e(and)h(SSD/RF,)g |
480360 |
< |
(as)f(w)n(ell)2042 5264 y(as)19 b(NVE)i(transp)r(ort)e(calculations)g |
480361 |
< |
(at)h(b)r(oth)h(self-consisten)n(t)e(and)2042 5359 y(exp)r(erimen)n |
480359 |
> |
3736 y(melting)f(sequences)f(for)g(b)r(oth)i(SSD/E)e(and)h(SSD/RF,)g |
480360 |
> |
(as)f(w)n(ell)2042 3831 y(as)19 b(NVE)i(transp)r(ort)e(calculations)g |
480361 |
> |
(at)h(b)r(oth)h(self-consisten)n(t)e(and)2042 3927 y(exp)r(erimen)n |
480362 |
|
(tal)j(densities.)35 b(Again,)24 b(the)f(results)g(come)f(from)h(\014v) |
480363 |
< |
n(e)p eop |
480363 |
> |
n(e)2042 4022 y(separate)37 b(sim)n(ulations)h(of)h(1024)e(particle)h |
480364 |
> |
(systems,)j(and)e(the)2042 4118 y(melting)23 b(sequences)f(w)n(ere)g |
480365 |
> |
(started)g(from)h(di\013eren)n(t)g(ice)g Fj(I)3844 4130 |
480366 |
> |
y Fi(h)3910 4118 y Fu(crys-)2042 4213 y(tals)30 b(constructed)f(as)h |
480367 |
> |
(stated)g(previously)-7 b(.)44 b(Lik)n(e)30 b(b)r(efore,)g(all)g(of) |
480368 |
> |
2042 4309 y(the)e(NPT)f(sim)n(ulations)f(w)n(ere)h(equilibrated)f(for)h |
480369 |
> |
(100)f(ps)h(b)r(efore)2042 4404 y(a)36 b(200)f(ps)h(data)g(collection)g |
480370 |
> |
(run,)i(and)e(they)h(used)f(the)h(previ-)2042 4500 y(ous)25 |
480371 |
> |
b(temp)r(erature's)g(\014nal)g(con\014guration)f(as)g(a)h(starting)g(p) |
480372 |
> |
r(oin)n(t.)2042 4595 y(All)e(of)g(the)g(NVE)g(sim)n(ulations)f(had)h |
480373 |
> |
(the)g(same)f(thermalization,)2042 4691 y(equilibration,)30 |
480374 |
> |
b(and)g(data)f(collection)h(times)g(stated)g(earlier)f(in)2042 |
480375 |
> |
4786 y(this)f(pap)r(er.)2125 4882 y(Figure)i(8)g(sho)n(ws)g(the)h |
480376 |
> |
(densit)n(y)f(pro\014le)h(for)f(the)h(SSD/E)f(w)n(a-)2042 |
480377 |
> |
4977 y(ter)j(mo)r(del)g(in)h(comparison)e(to)h(the)h(original)e(SSD)i |
480378 |
> |
(without)g(a)2042 5073 y(reaction)k(\014eld,)k(exp)r(erimen)n(t,)g(and) |
480379 |
> |
d(the)g(other)g(common)f(w)n(a-)2042 5168 y(ter)g(mo)r(dels)g |
480380 |
> |
(considered)f(previously)-7 b(.)67 b(The)39 b(calculated)e(den-)2042 |
480381 |
> |
5264 y(sities)d(ha)n(v)n(e)e(increased)h(signi\014can)n(tly)g(o)n(v)n |
480382 |
> |
(er)f(the)i(original)e(SSD)2042 5359 y(mo)r(del)c(and)g(matc)n(h)g(the) |
480383 |
> |
h(exp)r(erimen)n(tal)f(v)-5 b(alue)28 b(just)h(b)r(elo)n(w)f(298)p |
480384 |
> |
eop |
480385 |
|
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480386 |
|
8 7 bop 4043 -299 a Fu(8)-133 2245 y @beginspecial 44 |
480387 |
|
@llx 93 @lly 517 @urx 661 @ury 2409 @rwi @setspecial |
488877 |
|
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488878 |
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488879 |
|
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488880 |
< |
@endspecial -150 2415 a Fr(FIG.)34 b(9:)50 b(Comparison)34 |
488880 |
> |
@endspecial -150 2415 a Fr(FIG.)34 b(8:)50 b(Comparison)34 |
488881 |
|
b(of)h(densities)f(calculated)g(with)g(SSD/E)f(to)-150 |
488882 |
|
2502 y(SSD)c(without)i(a)g(reaction)g(\014eld,)h(TIP4P)1102 |
488883 |
|
2471 y Fc(19)1168 2502 y Fr(,)g(TIP3P)1446 2471 y Fc(19)1512 |
488886 |
|
y Fr(.)49 b(The)31 b(upp)r(er)f(plot)g(includes)h(error)g(bars,)i(and) |
488887 |
|
-150 2677 y(the)23 b(calculated)h(results)f(from)g(the)g(other)g |
488888 |
|
(references)h(w)n(ere)g(remo)n(v)n(ed)-150 2764 y(for)i(clarit)n(y)-6 |
488889 |
< |
b(.)-150 3044 y Fu(separate)37 b(sim)n(ulations)h(of)h(1024)e(particle) |
488890 |
< |
h(systems,)j(and)e(the)-150 3140 y(melting)23 b(sequences)f(w)n(ere)g |
488891 |
< |
(started)h(from)f(di\013eren)n(t)h(ice)g Fj(I)1652 3152 |
488892 |
< |
y Fi(h)1719 3140 y Fu(crys-)-150 3235 y(tals)30 b(constructed)g(as)f |
488893 |
< |
(stated)h(previously)-7 b(.)44 b(Lik)n(e)30 b(b)r(efore,)g(all)g(of) |
488894 |
< |
-150 3331 y(the)e(NPT)f(sim)n(ulations)f(w)n(ere)h(equilibrated)g(for)f |
488895 |
< |
(100)g(ps)i(b)r(efore)-150 3426 y(a)36 b(200)f(ps)h(data)g(collection)g |
488896 |
< |
(run,)i(and)f(they)f(used)g(the)h(previ-)-150 3522 y(ous)25 |
488897 |
< |
b(temp)r(erature's)g(\014nal)g(con\014guration)f(as)h(a)g(starting)f(p) |
488898 |
< |
r(oin)n(t.)-150 3617 y(All)f(of)g(the)g(NVE)g(sim)n(ulations)f(had)h |
497279 |
< |
(the)g(same)f(thermalization,)-150 3713 y(equilibration,)30 |
497280 |
< |
b(and)g(data)g(collection)f(times)h(stated)h(earlier)d(in)-150 |
497281 |
< |
3808 y(this)g(pap)r(er.)-67 3903 y(Figure)i(9)g(sho)n(ws)g(the)h |
497282 |
< |
(densit)n(y)g(pro\014le)f(for)g(the)h(SSD/E)g(w)n(a-)-150 |
497283 |
< |
3999 y(ter)i(mo)r(del)h(in)f(comparison)f(to)h(the)h(original)e(SSD)i |
497284 |
< |
(without)g(a)-150 4094 y(reaction)k(\014eld,)k(exp)r(erimen)n(t,)g(and) |
497285 |
< |
d(the)g(other)g(common)g(w)n(a-)-150 4190 y(ter)f(mo)r(dels)g |
497286 |
< |
(considered)f(previously)-7 b(.)68 b(The)38 b(calculated)g(den-)-150 |
497287 |
< |
4285 y(sities)c(ha)n(v)n(e)e(increased)h(signi\014can)n(tly)g(o)n(v)n |
497288 |
< |
(er)f(the)i(original)f(SSD)-150 4381 y(mo)r(del)28 b(and)h(matc)n(h)f |
497289 |
< |
(the)g(exp)r(erimen)n(tal)g(v)-5 b(alue)28 b(just)h(b)r(elo)n(w)f(298) |
497290 |
< |
-150 4476 y(K.)20 b(A)n(t)h(298)f(K,)g(the)h(densit)n(y)g(of)f(SSD/E)h |
497291 |
< |
(is)f(0.995)p Ff(\006)p Fu(0.001)d(g/cm)1833 4446 y Fn(3)1869 |
497292 |
< |
4476 y Fu(,)-150 4572 y(whic)n(h)k(compares)e(w)n(ell)h(with)i(the)f |
497293 |
< |
(exp)r(erimen)n(tal)f(v)-5 b(alue)21 b(of)f(0.997)-150 |
497294 |
< |
4667 y(g/cm)40 4637 y Fn(3)118 4667 y Fu(and)41 b(is)h(considerably)e |
497295 |
< |
(b)r(etter)i(than)f(the)h(SSD)h(v)-5 b(alue)-150 4763 |
497296 |
< |
y(of)43 b(0.967)p Ff(\006)p Fu(0.003)38 b(g/cm)635 4733 |
497297 |
< |
y Fn(3)671 4763 y Fu(.)82 b(The)43 b(increased)f(dip)r(ole)g(momen)n(t) |
497298 |
< |
-150 4858 y(in)33 b(SSD/E)f(has)f(help)r(ed)i(to)f(\015atten)h(out)f |
497299 |
< |
(the)h(curv)n(e)e(at)h(higher)-150 4954 y(temp)r(eratures,)25 |
488889 |
> |
b(.)-150 3044 y Fu(K.)20 b(A)n(t)h(298)f(K,)g(the)h(densit)n(y)g(of)f |
488890 |
> |
(SSD/E)h(is)f(0.995)p Ff(\006)p Fu(0.001)d(g/cm)1833 |
488891 |
> |
3014 y Fn(3)1869 3044 y Fu(,)-150 3140 y(whic)n(h)k(compares)e(w)n(ell) |
488892 |
> |
h(with)i(the)f(exp)r(erimen)n(tal)f(v)-5 b(alue)21 b(of)f(0.997)-150 |
488893 |
> |
3235 y(g/cm)40 3205 y Fn(3)118 3235 y Fu(and)41 b(is)h(considerably)e |
488894 |
> |
(b)r(etter)i(than)f(the)h(SSD)h(v)-5 b(alue)-150 3331 |
488895 |
> |
y(of)43 b(0.967)p Ff(\006)p Fu(0.003)38 b(g/cm)635 3300 |
488896 |
> |
y Fn(3)671 3331 y Fu(.)82 b(The)43 b(increased)f(dip)r(ole)g(momen)n(t) |
488897 |
> |
-150 3426 y(in)33 b(SSD/E)f(has)f(help)r(ed)i(to)f(\015atten)h(out)f |
488898 |
> |
(the)h(curv)n(e)e(at)h(higher)-150 3522 y(temp)r(eratures,)25 |
488899 |
|
b(only)g(the)h(impro)n(v)n(emen)n(t)e(is)i(marginal)e(at)h(b)r(est.) |
488900 |
< |
-150 5049 y(This)30 b(steep)f(drop)h(in)f(densities)h(is)g(due)g(to)f |
488901 |
< |
(the)h(dip)r(olar)f(rather)-150 5145 y(than)24 b(c)n(harge)e(based)i |
488900 |
> |
-150 3617 y(This)30 b(steep)f(drop)h(in)f(densities)h(is)g(due)g(to)f |
488901 |
> |
(the)h(dip)r(olar)f(rather)-150 3713 y(than)24 b(c)n(harge)e(based)i |
488902 |
|
(in)n(teractions)e(whic)n(h)i(deca)n(y)f(more)g(rapidly)-150 |
488903 |
< |
5240 y(at)k(longer)g(distances.)-67 5336 y(By)35 b(monitoring)g(Cp)g |
488904 |
< |
(throughout)g(these)g(sim)n(ulations,)i(the)2059 2245 |
488905 |
< |
y @beginspecial 44 @llx 93 @lly 517 @urx 661 @ury 2409 |
488906 |
< |
@rwi @setspecial |
488903 |
> |
3808 y(at)k(longer)g(distances.)-67 3903 y(By)35 b(monitoring)g(Cp)g |
488904 |
> |
(throughout)g(these)g(sim)n(ulations,)i(the)-150 3999 |
488905 |
> |
y(melting)42 b(transition)f(for)g(SSD/E)g(w)n(as)g(observ)n(ed)f(at)h |
488906 |
> |
(230)g(K,)-150 4094 y(ab)r(out)35 b(5)f(degrees)f(lo)n(w)n(er)g(than)i |
488907 |
> |
(SSD.)g(The)g(resulting)f(densit)n(y)-150 4190 y(maxim)n(um)41 |
488908 |
> |
b(is)g(lo)r(cated)g(at)g(240)f(K,)h(again)f(ab)r(out)h(5)g(degrees)-150 |
488909 |
> |
4285 y(lo)n(w)n(er)33 b(than)j(the)f(SSD)h(v)-5 b(alue)35 |
488910 |
> |
b(of)g(245)f(K.)g(Though)h(there)g(is)g(a)-150 4381 y(decrease)30 |
488911 |
> |
b(in)h(b)r(oth)h(of)f(these)h(v)-5 b(alues,)32 b(the)f(corrected)f |
488912 |
> |
(densities)-150 4476 y(near)d(ro)r(om)f(temp)r(erature)i(justify)g(the) |
488913 |
> |
g(mo)r(di\014cations)f(tak)n(en.)-67 4572 y(Figure)22 |
488914 |
> |
b(9)f(sho)n(ws)g(a)h(densit)n(y)g(comparison)f(b)r(et)n(w)n(een)h |
488915 |
> |
(SSD/RF)-150 4667 y(and)28 b(SSD)h(with)f(an)g(activ)n(e)f(reaction)g |
488916 |
> |
(\014eld.)39 b(Lik)n(e)27 b(in)h(the)h(sim)n(u-)-150 |
488917 |
> |
4763 y(lations)c(of)g(SSD/E,)g(the)h(densities)g(sho)n(w)e(a)h |
488918 |
> |
(dramatic)g(increase)-150 4858 y(o)n(v)n(er)34 b(normal)g(SSD.)i(A)n(t) |
488919 |
> |
g(298)e(K,)h(SSD/RF)h(has)f(a)g(densit)n(y)g(of)-150 |
488920 |
> |
4954 y(0.997)p Ff(\006)p Fu(0.001)g(g/cm)522 4924 y Fn(3)559 |
488921 |
> |
4954 y Fu(,)42 b(righ)n(t)d(in)h(line)f(with)h(exp)r(erimen)n(t)g(and) |
488922 |
> |
-150 5049 y(considerably)33 b(b)r(etter)h(than)g(the)h(SSD)g(v)-5 |
488923 |
> |
b(alue)34 b(of)g(0.941)p Ff(\006)p Fu(0.001)-150 5145 |
488924 |
> |
y(g/cm)40 5115 y Fn(3)76 5145 y Fu(.)55 b(The)33 b(melting)h(p)r(oin)n |
488925 |
> |
(t)g(is)f(observ)n(ed)f(at)h(240)f(K,)h(whic)n(h)-150 |
488926 |
> |
5240 y(is)j(5)g(degrees)g(lo)n(w)n(er)e(than)j(SSD)g(with)g(a)f |
488927 |
> |
(reaction)g(\014eld,)j(and)-150 5336 y(the)e(densit)n(y)g(maxim)n(um)g |
488928 |
> |
(at)g(255)f(K,)h(again)f(5)g(degrees)g(lo)n(w)n(er)2059 |
488929 |
> |
2245 y @beginspecial 44 @llx 93 @lly 517 @urx 661 @ury |
488930 |
> |
2409 @rwi @setspecial |
488931 |
|
%%BeginDocument: ssdrfcompare.epsi |
488932 |
|
%!PS-Adobe-2.0 EPSF-1.2 |
488933 |
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%%Title: ssdrfcompare.ps |
497483 |
|
%%EOF |
497484 |
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497485 |
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497486 |
< |
@endspecial 2042 2415 a Fr(FIG.)23 b(10:)34 b(Comparison)23 |
497487 |
< |
b(of)g(densities)h(calculated)f(with)g(SSD/RF)f(to)2042 |
497488 |
< |
2502 y(SSD)i(with)i(a)g(reaction)g(\014eld,)g(TIP4P)3157 |
497486 |
> |
@endspecial 2042 2415 a Fr(FIG.)28 b(9:)38 b(Comparison)28 |
497487 |
> |
b(of)g(densities)g(calculated)h(with)e(SSD/RF)g(to)2042 |
497488 |
> |
2502 y(SSD)d(with)i(a)g(reaction)g(\014eld,)g(TIP4P)3157 |
497489 |
|
2471 y Fc(19)3223 2502 y Fr(,)g(TIP3P)3495 2471 y Fc(19)3561 |
497490 |
|
2502 y Fr(,)g(SPC/E)3848 2471 y Fc(20)3914 2502 y Fr(,)f(and)2042 |
497491 |
|
2590 y(Exp)r(erimen)n(t)2435 2558 y Fc(21)2498 2590 y |
497492 |
|
Fr(.)55 b(The)32 b(upp)r(er)f(plot)i(includes)f(error)h(bars,)i(and)c |
497493 |
|
(the)2042 2677 y(calculated)26 b(results)f(from)g(the)f(other)h |
497494 |
|
(references)h(w)n(ere)g(remo)n(v)n(ed)d(for)2042 2764 |
497495 |
< |
y(clarit)n(y)-6 b(.)2042 3044 y Fu(melting)42 b(transition)f(for)g |
497496 |
< |
(SSD/E)g(w)n(as)g(observ)n(ed)f(at)h(230)f(K,)2042 3140 |
497497 |
< |
y(ab)r(out)34 b(5)g(degrees)g(lo)n(w)n(er)f(than)h(SSD.)i(The)e |
497498 |
< |
(resulting)g(densit)n(y)2042 3235 y(maxim)n(um)41 b(is)g(lo)r(cated)g |
497499 |
< |
(at)g(240)f(K,)h(again)f(ab)r(out)h(5)g(degrees)2042 |
497500 |
< |
3331 y(lo)n(w)n(er)33 b(than)i(the)h(SSD)g(v)-5 b(alue)35 |
497501 |
< |
b(of)g(245)e(K.)i(Though)g(there)g(is)g(a)2042 3426 y(decrease)30 |
505879 |
< |
b(in)h(b)r(oth)h(of)f(these)h(v)-5 b(alues,)32 b(the)f(corrected)f |
505880 |
< |
(densities)2042 3522 y(near)d(ro)r(om)f(temp)r(erature)h(justify)i(the) |
505881 |
< |
f(mo)r(di\014cations)f(tak)n(en.)2125 3617 y(Figure)70 |
505882 |
< |
b(10)g(sho)n(ws)g(a)h(densit)n(y)g(comparison)e(b)r(et)n(w)n(een)2042 |
505883 |
< |
3713 y(SSD/RF)41 b(and)f(SSD)h(with)g(an)g(activ)n(e)e(reaction)h |
505884 |
< |
(\014eld.)76 b(Lik)n(e)2042 3808 y(in)35 b(the)g(sim)n(ulations)f(of)g |
505885 |
< |
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505886 |
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y(matic)26 b(increase)e(o)n(v)n(er)g(normal)h(SSD.)h(A)n(t)h(298)d(K,)h |
505887 |
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505888 |
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505889 |
< |
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505890 |
< |
y(p)r(erimen)n(t)28 b(and)g(considerably)e(b)r(etter)j(than)f(the)h |
505891 |
< |
(SSD)f(v)-5 b(alue)28 b(of)2042 4190 y(0.941)p Ff(\006)p |
505892 |
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Fu(0.001)34 b(g/cm)2713 4160 y Fn(3)2750 4190 y Fu(.)70 |
505893 |
< |
b(The)38 b(melting)h(p)r(oin)n(t)g(is)f(observ)n(ed)f(at)2042 |
505894 |
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4285 y(240)21 b(K,)i(whic)n(h)g(is)g(5)g(degrees)f(lo)n(w)n(er)f(than)i |
505895 |
< |
(SSD)h(with)g(a)e(reaction)2042 4381 y(\014eld,)h(and)e(the)g(densit)n |
505896 |
< |
(y)h(maxim)n(um)f(at)g(255)f(K,)h(again)f(5)h(degrees)2042 |
505897 |
< |
4476 y(lo)n(w)n(er)26 b(than)j(SSD.)g(The)f(densit)n(y)g(at)g(higher)g |
505898 |
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(temp)r(erature)g(still)2042 4572 y(drops)c(o\013)g(more)g(rapidly)g |
505899 |
< |
(than)h(the)g(c)n(harge)e(based)h(mo)r(dels)h(but)2042 |
505900 |
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4667 y(is)i(in)h(b)r(etter)g(agreemen)n(t)e(than)i(SSD/E.)2125 |
505901 |
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4763 y(The)e(reparameterization)e(of)i(the)g(SSD)h(w)n(ater)e(mo)r |
505902 |
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505903 |
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(applied)f(long-range)e(correc-)2042 4954 y(tion,)41 |
497495 |
> |
y(clarit)n(y)-6 b(.)2042 3044 y Fu(than)27 b(SSD.)h(The)f(densit)n(y)g |
497496 |
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497497 |
> |
y(o\013)i(more)g(rapidly)g(than)h(the)g(c)n(harge)e(based)h(mo)r(dels)g |
497498 |
> |
(but)h(is)g(in)2042 3235 y(b)r(etter)e(agreemen)n(t)e(than)i(SSD/E.) |
497499 |
> |
2125 3331 y(The)e(reparameterization)e(of)i(the)g(SSD)h(w)n(ater)e(mo)r |
497500 |
> |
(del,)i(b)r(oth)2042 3426 y(for)34 b(use)g(with)h(and)g(without)f(an)h |
497501 |
> |
(applied)f(long-range)e(correc-)2042 3522 y(tion,)41 |
497502 |
|
b(brough)n(t)c(the)i(densities)f(up)h(to)f(what)g(is)g(exp)r(ected)h |
497503 |
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497504 |
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497503 |
> |
(for)2042 3617 y(sim)n(ulating)f(liquid)i(w)n(ater.)70 |
497504 |
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497505 |
|
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497506 |
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497507 |
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497508 |
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5336 y(dep)r(endence)35 b(of)g(the)g(di\013usion)g(constan)n(t)f(of)g |
497509 |
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497506 |
> |
r(ort)e(b)r(e)j(main-)2042 3808 y(tained)f(or)f(impro)n(v)n(ed.)34 |
497507 |
> |
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497508 |
> |
3903 y(dep)r(endence)35 b(of)g(the)g(di\013usion)g(constan)n(t)f(of)g |
497509 |
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(SSD/E)h(to)f(SSD)2042 3999 y(without)41 b(an)f(activ)n(e)g(reaction)f |
497510 |
> |
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497511 |
> |
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497512 |
> |
f(calculated)2042 4190 y(densities)h(for)g(sup)r(er-co)r(oled)g(and)g |
497513 |
> |
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497514 |
> |
4285 y(plot,)35 b(the)f(di\013usion)g(constan)n(t)f(for)g(SSD/E)g(is)h |
497515 |
> |
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497516 |
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497517 |
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4476 y(than)39 b(exp)r(erimen)n(t)g(and)g(crosses)e(to)i(merge)f(with)i |
497518 |
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(SSD/E)e(at)2042 4572 y(high)24 b(temp)r(eratures.)35 |
497519 |
> |
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497520 |
> |
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497521 |
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497522 |
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497523 |
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497524 |
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g(SSD/E)f(don't)i(devi-)2042 4954 y(ate)h(as)f(m)n(uc)n(h)h(from)g(exp) |
497525 |
> |
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497526 |
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497527 |
> |
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497528 |
> |
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497529 |
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(plot.)64 b(The)37 b(di\013usion)2042 5240 y(constan)n(ts)27 |
497530 |
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b(for)h(SSD/E)g(trac)n(k)g(with)h(the)g(exp)r(erimen)n(tal)f(v)-5 |
497531 |
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9 8 bop 4043 -299 a Fu(9)-133 2393 y @beginspecial 63 |
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@llx 92 @lly 515 @urx 668 @ury 2409 @rwi @setspecial |
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@endspecial -150 2563 a Fr(FIG.)42 b(11:)66 b(Plots)42 |
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@endspecial -150 2563 a Fr(FIG.)42 b(10:)66 b(Plots)42 |
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b(of)g(the)f(di\013usion)g(constan)n(ts)g(calculated)h(from)-150 |
506031 |
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2650 y(SSD/E)36 b(and)g(SSD,)f(b)r(oth)h(without)h(a)f(reaction)i |
506032 |
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(\014eld)e(along)h(with)-150 2737 y(exp)r(erimen)n(tal)e(results)i |
506036 |
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(calculated)h(from)f(the)f(NPT)h(sim)n(ula-)-150 2912 |
506037 |
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506038 |
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506039 |
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b(calculated)h(densities.)-150 3279 y Fu(without)41 b(an)f(activ)n(e)g |
506040 |
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506041 |
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506042 |
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514422 |
< |
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514423 |
< |
3565 y(plot,)35 b(the)f(di\013usion)g(constan)n(t)f(for)g(SSD/E)g(is)h |
514424 |
< |
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514425 |
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514426 |
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514427 |
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514428 |
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514429 |
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514430 |
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514431 |
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514432 |
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4138 y(system)i(densit)n(y)-7 b(.)36 b(Since)26 b(the)g(densities)g(of) |
514433 |
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514434 |
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514435 |
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4329 y(the)f(exp)r(erimen)n(tal)g(trend)g(more)f(closely)-7 |
514436 |
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b(.)36 b(This)27 b(observ)-5 b(ation)26 b(is)-150 4425 |
514437 |
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514438 |
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514439 |
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514440 |
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514441 |
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514442 |
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514443 |
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514444 |
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506039 |
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b(calculated)h(densities.)-150 3279 y Fu(creasing)f(temp)r(erature.)36 |
506040 |
> |
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506041 |
> |
3374 y(ha)n(ving)g(densities)i(closer)e(to)h(exp)r(erimen)n(t,)h(and)f |
506042 |
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506044 |
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506045 |
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506046 |
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(e)e(reaction)h(\014eld.)79 b(In)-150 5188 y(the)39 b(upp)r(er)g(plot,) |
506044 |
> |
3565 y(In)36 b(\014gure)f(11,)i(the)f(di\013usion)g(constan)n(ts)f(for) |
506045 |
> |
g(SSD/RF)h(are)-150 3661 y(compared)k(with)j(SSD)f(with)g(an)g(activ)n |
506046 |
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(e)e(reaction)h(\014eld.)79 b(In)-150 3756 y(the)39 b(upp)r(er)g(plot,) |
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506048 |
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5284 y(results)27 b(incredibly)g(w)n(ell,)g(iden)n(tical)h(within)g |
506049 |
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(error)d(throughout)-150 5379 y(the)f(temp)r(erature)f(range)g(and)g |
506050 |
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(only)h(sho)n(wing)e(a)i(sligh)n(t)f(increas-)2059 2393 |
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y @beginspecial 63 @llx 92 @lly 515 @urx 668 @ury 2409 |
506052 |
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@rwi @setspecial |
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> |
3852 y(results)27 b(incredibly)g(w)n(ell,)g(iden)n(tical)h(within)g |
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(error)d(throughout)-150 3947 y(the)f(temp)r(erature)f(range)g(and)g |
506050 |
> |
(only)h(sho)n(wing)e(a)i(sligh)n(t)f(increas-)-150 4043 |
506051 |
> |
y(ing)g(trend)g(at)g(higher)g(temp)r(eratures.)34 b(SSD)24 |
506052 |
> |
b(also)e(trac)n(ks)g(exp)r(er-)-150 4138 y(imen)n(t)35 |
506053 |
> |
b(w)n(ell,)h(only)e(it)h(tends)g(to)f(di\013use)h(a)f(little)i(more)d |
506054 |
> |
(slo)n(wly)-150 4234 y(at)f(lo)n(w)g(temp)r(eratures)g(and)g(deviates)g |
506055 |
> |
(to)g(di\013use)h(to)r(o)f(rapidly)-150 4329 y(at)26 |
506056 |
> |
b(high)h(temp)r(eratures.)35 b(As)27 b(w)n(as)e(stated)i(in)f(the)h |
506057 |
> |
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506058 |
> |
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506059 |
> |
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506060 |
> |
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506061 |
> |
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506062 |
> |
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506063 |
> |
4807 y(exp)r(erimen)n(t.)42 b(This)30 b(is)f(again)f(emphasized)h(in)h |
506064 |
> |
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506065 |
> |
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506066 |
> |
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506067 |
> |
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506068 |
> |
b(need)g(for)g(a)f(lo)n(w)n(er)g(densit)n(y)g(at)h(the)h(sp)r |
506069 |
> |
(eci\014ed)f(temp)r(erature.)2059 2393 y @beginspecial |
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> |
63 @llx 92 @lly 515 @urx 668 @ury 2409 @rwi @setspecial |
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@endspecial 2042 2563 a Fr(FIG.)41 b(12:)66 b(Plots)43 |
514553 |
> |
@endspecial 2042 2563 a Fr(FIG.)41 b(11:)66 b(Plots)43 |
514554 |
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b(of)f(the)e(di\013usion)i(constan)n(ts)f(calculated)h(from)2042 |
514555 |
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2650 y(SSD/RF)31 b(and)i(SSD,)e(b)r(oth)i(with)g(an)f(activ)n(e)h |
514556 |
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514559 |
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2824 y(The)27 b(upp)r(er)g(plot)g(is)h(at)f(densities)h(calculated)g |
514560 |
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514561 |
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514562 |
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2999 y(exp)r(erimen)n(tally)g(calculated)h(densities.)2042 |
514563 |
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3279 y Fu(ing)d(trend)g(at)g(higher)f(temp)r(eratures.)35 |
514564 |
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514565 |
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514566 |
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514567 |
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514568 |
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514569 |
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514570 |
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514571 |
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514573 |
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514574 |
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514575 |
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514576 |
< |
(the)h(lo)n(w)n(er)e(plot,)2042 4138 y(where)c(SSD/RF)i(trac)n(ks)e |
514577 |
< |
(the)h(exp)r(erimen)n(tal)g(di\013usion)g(exactly)2042 |
514578 |
< |
4234 y(while)20 b(SSD's)g(di\013usion)g(constan)n(ts)e(are)h(sligh)n |
514579 |
< |
(tly)g(to)r(o)g(lo)n(w)g(due)h(to)2042 4329 y(its)26 |
514580 |
< |
b(need)g(for)f(a)h(lo)n(w)n(er)e(densit)n(y)i(at)g(the)g(sp)r |
514581 |
< |
(eci\014ed)h(temp)r(erature.)2508 4605 y Fo(E.)88 b(Additional)32 |
514582 |
< |
b(Observ)-5 b(ations)2125 4819 y Fu(While)45 b(p)r(erforming)f(the)g |
514583 |
< |
(melting)h(sequences)f(of)g(SSD/E,)2042 4914 y(some)29 |
514584 |
< |
b(in)n(teresting)g(observ)-5 b(ations)28 b(w)n(ere)h(made.)43 |
514585 |
< |
b(After)30 b(melting)2042 5010 y(at)k(230)f(K,)h(t)n(w)n(o)g(of)g(the)h |
514586 |
< |
(systems)f(underw)n(en)n(t)g(crystallization)2042 5105 |
514587 |
< |
y(ev)n(en)n(ts)23 b(near)h(245)f(K.)h(As)g(the)h(heating)f(pro)r(cess)f |
514588 |
< |
(con)n(tin)n(ued,)i(the)2042 5201 y(t)n(w)n(o)c(systems)g(remained)g |
514589 |
< |
(crystalline)f(un)n(til)i(\014nally)f(melting)h(b)r(e-)2042 |
514590 |
< |
5296 y(t)n(w)n(een)32 b(320)g(and)g(330)f(K.)i(These)f(sim)n(ulations)g |
514591 |
< |
(w)n(ere)g(excluded)2042 5392 y(from)k(the)g(data)g(set)g(sho)n(wn)f |
514592 |
< |
(in)h(\014gure)g(9)g(and)f(replaced)h(with)p eop |
514562 |
> |
2999 y(exp)r(erimen)n(tally)g(calculated)h(densities.)2508 |
514563 |
> |
3279 y Fo(E.)88 b(Additional)32 b(Observ)-5 b(ations)2125 |
514564 |
> |
3493 y Fu(While)45 b(p)r(erforming)f(the)g(melting)h(sequences)f(of)g |
514565 |
> |
(SSD/E,)2042 3588 y(some)29 b(in)n(teresting)g(observ)-5 |
514566 |
> |
b(ations)28 b(w)n(ere)h(made.)43 b(After)30 b(melting)2042 |
514567 |
> |
3683 y(at)k(230)f(K,)h(t)n(w)n(o)g(of)g(the)h(systems)f(underw)n(en)n |
514568 |
> |
(t)g(crystallization)2042 3779 y(ev)n(en)n(ts)23 b(near)h(245)f(K.)h |
514569 |
> |
(As)g(the)h(heating)f(pro)r(cess)f(con)n(tin)n(ued,)i(the)2042 |
514570 |
> |
3874 y(t)n(w)n(o)c(systems)g(remained)g(crystalline)f(un)n(til)i |
514571 |
> |
(\014nally)f(melting)h(b)r(e-)2042 3970 y(t)n(w)n(een)32 |
514572 |
> |
b(320)g(and)g(330)f(K.)i(These)f(sim)n(ulations)g(w)n(ere)g(excluded) |
514573 |
> |
2042 4065 y(from)k(the)g(data)g(set)g(sho)n(wn)f(in)h(\014gure)g(8)g |
514574 |
> |
(and)f(replaced)h(with)2042 4161 y(t)n(w)n(o)f(additional)g(melting)g |
514575 |
> |
(sequences)g(that)h(did)g(not)f(undergo)2042 4256 y(this)j(anomalous)e |
514576 |
> |
(phase)h(transition,)i(while)f(this)g(crystalliza-)2042 |
514577 |
> |
4352 y(tion)27 b(ev)n(en)n(t)h(w)n(as)e(in)n(v)n(estigated)g |
514578 |
> |
(separately)-7 b(.)2125 4447 y(The)21 b(\014nal)g(con\014gurations)f |
514579 |
> |
(of)h(these)g(t)n(w)n(o)g(melting)g(sequences)2042 4543 |
514580 |
> |
y(sho)n(ws)d(an)h(expanded)f(zeolite-lik)n(e)g(crystal)h(structure)f |
514581 |
> |
(that)i(do)r(es)2042 4638 y(not)39 b(corresp)r(ond)e(to)i(an)n(y)f(kno) |
514582 |
> |
n(wn)h(form)f(of)h(ice.)71 b(F)-7 b(or)39 b(con)n(v)n(e-)2042 |
514583 |
> |
4734 y(nience)23 b(and)h(to)f(help)h(distinguish)g(it)g(from)f(the)h |
514584 |
> |
(exp)r(erimen)n(tally)2042 4829 y(observ)n(ed)32 b(forms)i(of)g(ice,)h |
514585 |
> |
(this)g(crystal)e(structure)g(will)i(hence-)2042 4925 |
514586 |
> |
y(forth)29 b(b)r(e)h(referred)e(to)h(as)g(ice-zero)f(\(ice)i(0\).)42 |
514587 |
> |
b(The)29 b(crystallinit)n(y)2042 5020 y(w)n(as)d(extensiv)n(e)g(enough) |
514588 |
> |
g(than)h(a)f(near)g(ideal)h(crystal)f(structure)2042 |
514589 |
> |
5116 y(could)31 b(b)r(e)h(obtained.)49 b(Figure)31 b(12)f(sho)n(ws)h |
514590 |
> |
(the)h(rep)r(eating)e(crys-)2042 5211 y(tal)37 b(structure)f(of)h(a)g |
514591 |
> |
(t)n(ypical)f(crystal)g(at)h(5)g(K.)f(The)i(unit)f(cell)2042 |
514592 |
> |
5307 y(con)n(tains)27 b(eigh)n(t)i(molecules,)f(and)g(\014gure)g(13)g |
514593 |
> |
(sho)n(ws)f(a)h(unit)h(cell)2042 5402 y(built)34 b(from)g(the)g(w)n |
514594 |
> |
(ater)f(particle)g(cen)n(ter)h(of)g(masses)e(that)j(can)p |
514595 |
> |
eop |
514596 |
|
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514597 |
|
10 9 bop 4001 -299 a Fu(10)-133 1529 y @beginspecial |
514598 |
|
0 @llx 0 @lly 1169 @urx 987 @ury 2409 @rwi @setspecial |
619537 |
|
%%EOF |
619538 |
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|
619539 |
|
%%EndDocument |
619540 |
< |
@endspecial -150 1699 a Fr(FIG.)26 b(13:)35 b(Crystal)26 |
619540 |
> |
@endspecial -150 1699 a Fr(FIG.)26 b(12:)35 b(Crystal)26 |
619541 |
|
b(structure)e(of)i(an)g(ice)f(0)h(lattice)g(sho)n(wn)g(from)f(the)-150 |
619542 |
< |
1787 y(\(001\))i(face.)-150 2071 y Fu(t)n(w)n(o)35 b(additional)g |
619543 |
< |
(melting)g(sequences)g(that)h(did)g(not)g(undergo)-150 |
627925 |
< |
2166 y(this)i(anomalous)e(phase)h(transition,)j(while)d(this)h |
627926 |
< |
(crystalliza-)-150 2262 y(tion)28 b(ev)n(en)n(t)f(w)n(as)f(in)n(v)n |
627927 |
< |
(estigated)h(separately)-7 b(.)-67 2357 y(The)21 b(\014nal)g |
627928 |
< |
(con\014gurations)f(of)h(these)g(t)n(w)n(o)g(melting)g(sequences)-150 |
627929 |
< |
2453 y(sho)n(ws)d(an)h(expanded)g(zeolite-lik)n(e)f(crystal)g |
627930 |
< |
(structure)g(that)i(do)r(es)-150 2548 y(not)39 b(corresp)r(ond)e(to)i |
627931 |
< |
(an)n(y)g(kno)n(wn)f(form)h(of)g(ice.)71 b(F)-7 b(or)38 |
627932 |
< |
b(con)n(v)n(e-)-150 2644 y(nience)24 b(and)f(to)g(help)h(distinguish)g |
627933 |
< |
(it)g(from)f(the)h(exp)r(erimen)n(tally)-150 2739 y(observ)n(ed)32 |
627934 |
< |
b(forms)i(of)g(ice,)i(this)e(crystal)f(structure)g(will)i(hence-)-150 |
627935 |
< |
2835 y(forth)29 b(b)r(e)h(referred)e(to)i(as)e(ice-zero)g(\(ice)i(0\).) |
627936 |
< |
42 b(The)29 b(crystallinit)n(y)-150 2930 y(w)n(as)d(extensiv)n(e)g |
627937 |
< |
(enough)g(than)h(a)g(near)f(ideal)g(crystal)g(structure)-150 |
627938 |
< |
3026 y(could)31 b(b)r(e)h(obtained.)49 b(Figure)31 b(13)f(sho)n(ws)h |
627939 |
< |
(the)h(rep)r(eating)f(crys-)-150 3121 y(tal)37 b(structure)f(of)h(a)g |
627940 |
< |
(t)n(ypical)g(crystal)e(at)i(5)g(K.)g(The)g(unit)g(cell)-150 |
627941 |
< |
3217 y(con)n(tains)28 b(eigh)n(t)g(molecules,)g(and)g(\014gure)g(14)g |
627942 |
< |
(sho)n(ws)f(a)h(unit)h(cell)-150 3312 y(built)35 b(from)e(the)h(w)n |
627943 |
< |
(ater)f(particle)h(cen)n(ter)f(of)h(masses)f(that)h(can)-150 |
627944 |
< |
3408 y(b)r(e)i(used)f(to)g(construct)g(a)g(rep)r(eating)f(lattice,)j |
627945 |
< |
(similar)e(to)g(\014g-)-150 3503 y(ure)28 b(13.)38 b(Eac)n(h)27 |
627946 |
< |
b(molecule)h(is)h(h)n(ydrogen)d(b)r(onded)j(to)f(four)g(other)-150 |
627947 |
< |
3598 y(w)n(ater)c(molecules;)h(ho)n(w)n(ev)n(er,)e(the)i(h)n(ydrogen)e |
627948 |
< |
(b)r(onds)i(are)e(\015exed)-150 3694 y(rather)31 b(than)h(p)r(erfectly) |
627949 |
< |
g(straigh)n(t.)49 b(This)32 b(results)g(in)g(a)g(sk)n(ew)n(ed)-150 |
627950 |
< |
3789 y(tetrahedral)c(geometry)g(ab)r(out)h(the)h(cen)n(tral)e |
627951 |
< |
(molecule.)42 b(Lo)r(ok-)-150 3885 y(ing)36 b(bac)n(k)f(at)h(\014gure)g |
627952 |
< |
(8,)i(it)e(is)h(easy)e(to)h(see)g(ho)n(w)f(these)h(\015exed)-150 |
627953 |
< |
3980 y(h)n(ydrogen)20 b(b)r(onds)i(are)f(allo)n(w)n(ed)f(in)i(that)g |
627954 |
< |
(the)g(attractiv)n(e)f(regions)-150 4076 y(are)30 b(conical)f(in)i |
627955 |
< |
(shap)r(e,)g(with)g(the)g(greatest)f(attraction)f(in)i(the)-150 |
627956 |
< |
4171 y(cen)n(tral)e(region.)44 b(Though)30 b(not)g(ideal,)h(these)g |
627957 |
< |
(\015exed)f(h)n(ydrogen)-150 4267 y(b)r(onds)e(are)f(fa)n(v)n(orable)f |
627958 |
< |
(enough)h(to)h(stabilize)g(an)g(en)n(tire)g(crystal)-150 |
627959 |
< |
4362 y(generated)22 b(around)h(them.)36 b(In)24 b(fact,)h(the)f(imp)r |
627960 |
< |
(erfect)g(ice)f(0)h(crys-)-150 4458 y(tals)e(w)n(ere)g(so)f(stable)h |
627961 |
< |
(that)h(they)g(melted)g(at)f(greater)f(than)h(ro)r(om)-150 |
627962 |
< |
4553 y(temp)r(erature.)-67 4649 y(The)29 b(initial)g(sim)n(ulations)e |
627963 |
< |
(indicated)i(that)g(ice)f(0)h(is)f(the)h(pre-)-150 4744 |
627964 |
< |
y(ferred)37 b(ice)g(structure)f(for)h(at)g(least)g(SSD/E.)g(T)-7 |
627965 |
< |
b(o)37 b(v)n(erify)f(this,)-150 4840 y(a)h(comparison)f(w)n(as)g(made)i |
627966 |
< |
(b)r(et)n(w)n(een)f(near)g(ideal)g(crystals)f(of)-150 |
627967 |
< |
4935 y(ice)24 b Fj(I)7 4947 y Fi(h)50 4935 y Fu(,)h(ice)f |
627968 |
< |
Fj(I)255 4947 y Fi(c)289 4935 y Fu(,)h(and)f(ice)f(0)h(at)g(constan)n |
627969 |
< |
(t)f(pressure)f(with)j(SSD/E,)-150 5031 y(SSD/RF,)e(and)g(SSD.)g(Near)f |
627970 |
< |
(ideal)h(v)n(ersions)d(of)j(the)g(three)f(t)n(yp)r(es)-150 |
627971 |
< |
5126 y(of)32 b(crystals)f(w)n(ere)g(co)r(oled)g(to)64 |
627972 |
< |
b(1)31 b(K,)h(and)g(the)g(p)r(oten)n(tial)g(ener-)-150 |
627973 |
< |
5222 y(gies)25 b(of)g(eac)n(h)g(w)n(ere)f(compared)h(using)g(all)g |
627974 |
< |
(three)g(w)n(ater)f(mo)r(dels.)-150 5317 y(With)d(ev)n(ery)d(w)n(ater)h |
627975 |
< |
(mo)r(del,)i(ice)f(0)f(turned)h(out)g(to)g(ha)n(v)n(e)e(the)i(lo)n(w-) |
627976 |
< |
-150 5412 y(est)31 b(p)r(oten)n(tial)h(energy:)43 b(5\045)31 |
627977 |
< |
b(lo)n(w)n(er)f(than)h Fj(I)1239 5424 y Fi(h)1314 5412 |
627978 |
< |
y Fu(with)h(SSD,)g(6.5\045)2295 1131 y @beginspecial |
627979 |
< |
0 @llx 0 @lly 232 @urx 196 @ury 1842 @rwi @setspecial |
619542 |
> |
1787 y(\(001\))i(face.)103 3219 y @beginspecial 0 @llx |
619543 |
> |
0 @lly 232 @urx 196 @ury 1842 @rwi @setspecial |
619544 |
|
%%BeginDocument: ice0cell.eps |
619545 |
|
%!PS-Adobe-3.1 EPSF-3.0 |
619546 |
|
%%Title: ice0cell.eps |
627331 |
|
%AI9_PrivateDataEnd |
627332 |
|
|
627333 |
|
%%EndDocument |
627334 |
< |
@endspecial 2042 1301 a Fr(FIG.)c(14:)39 b(Simple)27 |
627335 |
< |
b(unit)h(cell)g(for)h(constructing)f(ice)h(0.)41 b(In)27 |
627336 |
< |
b(this)h(cell,)2042 1389 y Fq(c)e Fr(is)g(equal)g(to)f(0)p |
627337 |
< |
Fq(:)p Fr(4714)20 b Fa(\002)d Fq(a)p Fr(,)25 b(and)h(a)g(t)n(ypical)f |
627338 |
< |
(v)l(alue)h(for)g Fq(a)f Fr(is)i(8.25)3956 1376 y(\027)3956 |
627339 |
< |
1389 y(A.)2042 1669 y Fu(lo)n(w)n(er)g(with)h(SSD/E,)h(and)f(7.5\045)f |
627340 |
< |
(lo)n(w)n(er)g(with)i(SSD/RF.)g(In)f(all)2042 1764 y(three)35 |
627341 |
< |
b(of)g(these)h(w)n(ater)e(mo)r(dels,)k(ice)d Fj(I)3302 |
627342 |
< |
1776 y Fi(c)3372 1764 y Fu(w)n(as)g(observ)n(ed)e(to)j(b)r(e)2042 |
627343 |
< |
1860 y(2\045)23 b(less)g(stable)h(than)g(ice)f Fj(I)2908 |
627344 |
< |
1872 y Fi(h)2952 1860 y Fu(.)36 b(In)23 b(addition)h(to)g(ha)n(ving)e |
627345 |
< |
(the)i(lo)n(w-)2042 1955 y(est)j(p)r(oten)n(tial)h(energy)-7 |
627334 |
> |
@endspecial -150 3389 a(FIG.)h(13:)40 b(Simple)27 b(unit)g(cell)i(for) |
627335 |
> |
f(constructing)g(ice)h(0.)41 b(In)27 b(this)h(cell,)-150 |
627336 |
> |
3476 y Fq(c)e Fr(is)g(equal)g(to)g(0)p Fq(:)p Fr(4714)19 |
627337 |
> |
b Fa(\002)e Fq(a)p Fr(,)25 b(and)h(a)g(t)n(ypical)f(v)l(alue)h(for)g |
627338 |
> |
Fq(a)g Fr(is)g(8.25)1764 3463 y(\027)1764 3476 y(A.)-150 |
627339 |
> |
3756 y Fu(b)r(e)36 b(used)f(to)g(construct)g(a)g(rep)r(eating)f |
627340 |
> |
(lattice,)j(similar)e(to)g(\014g-)-150 3852 y(ure)28 |
627341 |
> |
b(12.)38 b(Eac)n(h)27 b(molecule)h(is)h(h)n(ydrogen)d(b)r(onded)j(to)f |
627342 |
> |
(four)g(other)-150 3947 y(w)n(ater)c(molecules;)h(ho)n(w)n(ev)n(er,)e |
627343 |
> |
(the)i(h)n(ydrogen)e(b)r(onds)i(are)e(\015exed)-150 4043 |
627344 |
> |
y(rather)31 b(than)h(p)r(erfectly)g(straigh)n(t.)49 b(This)32 |
627345 |
> |
b(results)g(in)g(a)g(sk)n(ew)n(ed)-150 4138 y(tetrahedral)c(geometry)g |
627346 |
> |
(ab)r(out)h(the)h(cen)n(tral)e(molecule.)42 b(Lo)r(ok-)-150 |
627347 |
> |
4234 y(ing)36 b(bac)n(k)f(at)h(\014gure)g(7,)i(it)e(is)h(easy)e(to)h |
627348 |
> |
(see)g(ho)n(w)f(these)h(\015exed)-150 4329 y(h)n(ydrogen)20 |
627349 |
> |
b(b)r(onds)i(are)f(allo)n(w)n(ed)f(in)i(that)g(the)g(attractiv)n(e)f |
627350 |
> |
(regions)-150 4425 y(are)30 b(conical)f(in)i(shap)r(e,)g(with)g(the)g |
627351 |
> |
(greatest)f(attraction)f(in)i(the)-150 4520 y(cen)n(tral)e(region.)44 |
627352 |
> |
b(Though)30 b(not)g(ideal,)h(these)g(\015exed)f(h)n(ydrogen)-150 |
627353 |
> |
4615 y(b)r(onds)e(are)f(fa)n(v)n(orable)f(enough)h(to)h(stabilize)g(an) |
627354 |
> |
g(en)n(tire)g(crystal)-150 4711 y(generated)22 b(around)h(them.)36 |
627355 |
> |
b(In)24 b(fact,)h(the)f(imp)r(erfect)g(ice)f(0)h(crys-)-150 |
627356 |
> |
4806 y(tals)e(w)n(ere)g(so)f(stable)h(that)h(they)g(melted)g(at)f |
627357 |
> |
(greater)f(than)h(ro)r(om)-150 4902 y(temp)r(erature.)-67 |
627358 |
> |
4997 y(The)29 b(initial)g(sim)n(ulations)e(indicated)i(that)g(ice)f(0)h |
627359 |
> |
(is)f(the)h(pre-)-150 5093 y(ferred)37 b(ice)g(structure)f(for)h(at)g |
627360 |
> |
(least)g(SSD/E.)g(T)-7 b(o)37 b(v)n(erify)f(this,)-150 |
627361 |
> |
5188 y(a)h(comparison)f(w)n(as)g(made)i(b)r(et)n(w)n(een)f(near)g |
627362 |
> |
(ideal)g(crystals)f(of)-150 5284 y(ice)24 b Fj(I)7 5296 |
627363 |
> |
y Fi(h)50 5284 y Fu(,)h(ice)f Fj(I)255 5296 y Fi(c)289 |
627364 |
> |
5284 y Fu(,)h(and)f(ice)f(0)h(at)g(constan)n(t)f(pressure)f(with)j |
627365 |
> |
(SSD/E,)-150 5379 y(SSD/RF,)e(and)g(SSD.)g(Near)f(ideal)h(v)n(ersions)d |
627366 |
> |
(of)j(the)g(three)f(t)n(yp)r(es)2042 -83 y(of)32 b(crystals)e(w)n(ere)h |
627367 |
> |
(co)r(oled)h(to)64 b(1)31 b(K,)h(and)g(the)g(p)r(oten)n(tial)g(ener-) |
627368 |
> |
2042 12 y(gies)25 b(of)g(eac)n(h)g(w)n(ere)f(compared)g(using)h(all)h |
627369 |
> |
(three)f(w)n(ater)f(mo)r(dels.)2042 108 y(With)c(ev)n(ery)f(w)n(ater)g |
627370 |
> |
(mo)r(del,)i(ice)f(0)f(turned)h(out)g(to)g(ha)n(v)n(e)e(the)i(lo)n(w-) |
627371 |
> |
2042 203 y(est)31 b(p)r(oten)n(tial)g(energy:)44 b(5\045)31 |
627372 |
> |
b(lo)n(w)n(er)e(than)j Fj(I)3431 215 y Fi(h)3506 203 |
627373 |
> |
y Fu(with)g(SSD,)g(6.5\045)2042 299 y(lo)n(w)n(er)27 |
627374 |
> |
b(with)h(SSD/E,)h(and)f(7.5\045)f(lo)n(w)n(er)g(with)i(SSD/RF.)g(In)f |
627375 |
> |
(all)2042 394 y(three)35 b(of)g(these)h(w)n(ater)e(mo)r(dels,)k(ice)d |
627376 |
> |
Fj(I)3302 406 y Fi(c)3372 394 y Fu(w)n(as)g(observ)n(ed)e(to)j(b)r(e) |
627377 |
> |
2042 490 y(2\045)23 b(less)g(stable)h(than)g(ice)f Fj(I)2908 |
627378 |
> |
502 y Fi(h)2952 490 y Fu(.)36 b(In)23 b(addition)h(to)g(ha)n(ving)e |
627379 |
> |
(the)i(lo)n(w-)2042 585 y(est)j(p)r(oten)n(tial)h(energy)-7 |
627380 |
|
b(,)26 b(ice)i(0)f(w)n(as)g(the)h(most)f(expanded)g(of)h(the)2042 |
627381 |
< |
2051 y(three)i(ice)h(crystals,)60 b(5\045)31 b(less)f(dense)g(than)h |
627382 |
< |
(ice)g Fj(I)3633 2063 y Fi(h)3707 2051 y Fu(with)g(all)f(of)2042 |
627383 |
< |
2146 y(the)h(w)n(ater)f(mo)r(dels.)47 b(In)31 b(all)g(three)g(w)n(ater) |
627384 |
< |
f(mo)r(dels,)i(ice)f Fj(I)3887 2158 y Fi(c)3952 2146 |
627385 |
< |
y Fu(w)n(as)2042 2242 y(observ)n(ed)26 b(to)h(b)r(e)56 |
627386 |
< |
b(2\045)27 b(more)g(dense)h(than)f(ice)h Fj(I)3553 2254 |
627387 |
< |
y Fi(h)3596 2242 y Fu(.)2125 2337 y(In)c(addition)g(to)g(the)h(lo)n(w)e |
627388 |
< |
(temp)r(erature)h(comparisons,)f(melt-)2042 2433 y(ing)38 |
627389 |
< |
b(sequences)g(w)n(ere)f(p)r(erformed)i(with)g(ice)f(0)g(as)g(the)h |
627390 |
< |
(initial)2042 2528 y(con\014guration)19 b(using)h(SSD/E,)h(SSD/RF,)g |
627391 |
< |
(and)g(SSD)g(b)r(oth)h(with)2042 2624 y(and)k(without)h(a)f(reaction)f |
627392 |
< |
(\014eld.)36 b(The)27 b(melting)f(transitions)g(for)2042 |
627393 |
< |
2719 y(b)r(oth)20 b(SSD/E)g(and)f(SSD)i(without)f(a)g(reaction)e |
627394 |
< |
(\014eld)j(o)r(ccurred)d(at)2042 2814 y(temp)r(erature)29 |
627395 |
< |
b(in)g(excess)g(of)g(375)f(K.)h(SSD/RF)h(and)g(SSD)g(with)2042 |
627396 |
< |
2910 y(a)c(reaction)f(\014eld)i(had)f(more)g(reasonable)e(melting)j |
627397 |
< |
(transitions,)2042 3005 y(do)n(wn)h(near)f(325)g(K.)h(These)g(melting)h |
627398 |
< |
(p)r(oin)n(t)g(observ)-5 b(ations)26 b(em-)2042 3101 |
627399 |
< |
y(phasize)34 b(ho)n(w)h(preferred)f(this)h(crystal)f(structure)h(is)g |
627400 |
< |
(o)n(v)n(er)e(the)2042 3196 y(most)27 b(common)h(t)n(yp)r(es)f(of)h |
627401 |
< |
(ice)g(when)g(using)f(these)h(single)f(p)r(oin)n(t)2042 |
627402 |
< |
3292 y(w)n(ater)f(mo)r(dels.)2125 3387 y(Recognizing)c(that)i(the)h(ab) |
627403 |
< |
r(o)n(v)n(e)d(tests)i(sho)n(w)f(ice)h(0)f(to)h(b)r(e)g(b)r(oth)2042 |
627404 |
< |
3483 y(the)32 b(most)f(stable)h(and)f(lo)n(w)n(est)g(densit)n(y)g |
627405 |
< |
(crystal)g(structure)g(for)2042 3578 y(these)26 b(single)g(p)r(oin)n(t) |
627406 |
< |
h(w)n(ater)f(mo)r(dels,)h(it)g(is)f(in)n(teresting)g(to)g(sp)r(ec-)2042 |
627407 |
< |
3674 y(ulate)c(on)g(the)g(fa)n(v)n(orabilit)n(y)e(of)i(this)h(crystal)e |
627408 |
< |
(structure)g(with)i(the)2042 3769 y(di\013eren)n(t)33 |
627409 |
< |
b(c)n(harge)e(based)i(mo)r(dels.)53 b(As)33 b(a)f(quic)n(k)h(test,)i |
627410 |
< |
(these)e(3)2042 3865 y(crystal)28 b(t)n(yp)r(es)h(w)n(ere)f(con)n(v)n |
627411 |
< |
(erted)f(from)i(SSD)h(t)n(yp)r(e)f(particles)f(to)2042 |
627412 |
< |
3960 y(TIP3P)h(w)n(aters)h(and)h(read)f(in)n(to)h(CHARMM.)3527 |
627413 |
< |
3930 y Fn(30)3629 3960 y Fu(Iden)n(tical)f(en-)2042 4056 |
627414 |
< |
y(ergy)f(minimizations)i(w)n(ere)e(p)r(erformed)i(on)f(all)g(of)h |
627415 |
< |
(these)f(crys-)2042 4151 y(tals)36 b(to)g(compare)e(the)j(system)f |
627416 |
< |
(energies.)61 b(Again,)38 b(ice)e(0)f(w)n(as)2042 4247 |
627417 |
< |
y(observ)n(ed)23 b(to)i(ha)n(v)n(e)f(the)h(lo)n(w)n(est)f(total)h |
627418 |
< |
(system)g(energy)-7 b(.)35 b(The)25 b(to-)2042 4342 y(tal)c(energy)e |
627419 |
< |
(of)i(ice)g(0)f(w)n(as)41 b(2\045)21 b(lo)n(w)n(er)e(than)i(ice)g |
627420 |
< |
Fj(I)3543 4354 y Fi(h)3586 4342 y Fu(,)h(whic)n(h)f(w)n(as)f(in)2042 |
627421 |
< |
4438 y(turn)50 b(3\045)25 b(lo)n(w)n(er)e(than)i(ice)g |
627422 |
< |
Fj(I)2948 4450 y Fi(c)2983 4438 y Fu(.)36 b(F)-7 b(rom)24 |
627423 |
< |
b(these)h(initial)h(results,)f(w)n(e)2042 4533 y(w)n(ould)g(not)h(b)r |
627381 |
> |
681 y(three)i(ice)h(crystals,)60 b(5\045)31 b(less)f(dense)g(than)h |
627382 |
> |
(ice)g Fj(I)3633 693 y Fi(h)3707 681 y Fu(with)g(all)f(of)2042 |
627383 |
> |
776 y(the)h(w)n(ater)f(mo)r(dels.)47 b(In)31 b(all)g(three)g(w)n(ater)f |
627384 |
> |
(mo)r(dels,)i(ice)f Fj(I)3887 788 y Fi(c)3952 776 y Fu(w)n(as)2042 |
627385 |
> |
872 y(observ)n(ed)26 b(to)h(b)r(e)56 b(2\045)27 b(more)g(dense)h(than)f |
627386 |
> |
(ice)h Fj(I)3553 884 y Fi(h)3596 872 y Fu(.)2125 967 |
627387 |
> |
y(In)c(addition)g(to)g(the)h(lo)n(w)e(temp)r(erature)h(comparisons,)f |
627388 |
> |
(melt-)2042 1063 y(ing)38 b(sequences)g(w)n(ere)f(p)r(erformed)i(with)g |
627389 |
> |
(ice)f(0)g(as)g(the)h(initial)2042 1158 y(con\014guration)19 |
627390 |
> |
b(using)h(SSD/E,)h(SSD/RF,)g(and)g(SSD)g(b)r(oth)h(with)2042 |
627391 |
> |
1254 y(and)k(without)h(a)f(reaction)f(\014eld.)36 b(The)27 |
627392 |
> |
b(melting)f(transitions)g(for)2042 1349 y(b)r(oth)20 |
627393 |
> |
b(SSD/E)g(and)f(SSD)i(without)f(a)g(reaction)e(\014eld)j(o)r(ccurred)d |
627394 |
> |
(at)2042 1445 y(temp)r(erature)29 b(in)g(excess)g(of)g(375)f(K.)h |
627395 |
> |
(SSD/RF)h(and)g(SSD)g(with)2042 1540 y(a)c(reaction)f(\014eld)i(had)f |
627396 |
> |
(more)g(reasonable)e(melting)j(transitions,)2042 1636 |
627397 |
> |
y(do)n(wn)h(near)f(325)g(K.)h(These)g(melting)h(p)r(oin)n(t)g(observ)-5 |
627398 |
> |
b(ations)26 b(em-)2042 1731 y(phasize)34 b(ho)n(w)h(preferred)f(this)h |
627399 |
> |
(crystal)f(structure)h(is)g(o)n(v)n(er)e(the)2042 1826 |
627400 |
> |
y(most)27 b(common)h(t)n(yp)r(es)f(of)h(ice)g(when)g(using)f(these)h |
627401 |
> |
(single)f(p)r(oin)n(t)2042 1922 y(w)n(ater)f(mo)r(dels.)2125 |
627402 |
> |
2017 y(Recognizing)c(that)i(the)h(ab)r(o)n(v)n(e)d(tests)i(sho)n(w)f |
627403 |
> |
(ice)h(0)f(to)h(b)r(e)g(b)r(oth)2042 2113 y(the)32 b(most)f(stable)h |
627404 |
> |
(and)f(lo)n(w)n(est)g(densit)n(y)g(crystal)g(structure)g(for)2042 |
627405 |
> |
2208 y(these)26 b(single)g(p)r(oin)n(t)h(w)n(ater)f(mo)r(dels,)h(it)g |
627406 |
> |
(is)f(in)n(teresting)g(to)g(sp)r(ec-)2042 2304 y(ulate)c(on)g(the)g(fa) |
627407 |
> |
n(v)n(orabilit)n(y)e(of)i(this)h(crystal)e(structure)g(with)i(the)2042 |
627408 |
> |
2399 y(di\013eren)n(t)33 b(c)n(harge)e(based)i(mo)r(dels.)53 |
627409 |
> |
b(As)33 b(a)f(quic)n(k)h(test,)i(these)e(3)2042 2495 |
627410 |
> |
y(crystal)28 b(t)n(yp)r(es)h(w)n(ere)f(con)n(v)n(erted)f(from)i(SSD)h |
627411 |
> |
(t)n(yp)r(e)f(particles)f(to)2042 2590 y(TIP3P)h(w)n(aters)h(and)h |
627412 |
> |
(read)f(in)n(to)h(CHARMM.)3527 2560 y Fn(30)3629 2590 |
627413 |
> |
y Fu(Iden)n(tical)f(en-)2042 2686 y(ergy)f(minimizations)i(w)n(ere)e(p) |
627414 |
> |
r(erformed)i(on)f(all)g(of)h(these)f(crys-)2042 2781 |
627415 |
> |
y(tals)36 b(to)g(compare)e(the)j(system)f(energies.)61 |
627416 |
> |
b(Again,)38 b(ice)e(0)f(w)n(as)2042 2877 y(observ)n(ed)23 |
627417 |
> |
b(to)i(ha)n(v)n(e)f(the)h(lo)n(w)n(est)f(total)h(system)g(energy)-7 |
627418 |
> |
b(.)35 b(The)25 b(to-)2042 2972 y(tal)c(energy)e(of)i(ice)g(0)f(w)n(as) |
627419 |
> |
41 b(2\045)21 b(lo)n(w)n(er)e(than)i(ice)g Fj(I)3543 |
627420 |
> |
2984 y Fi(h)3586 2972 y Fu(,)h(whic)n(h)f(w)n(as)f(in)2042 |
627421 |
> |
3068 y(turn)50 b(3\045)25 b(lo)n(w)n(er)e(than)i(ice)g |
627422 |
> |
Fj(I)2948 3080 y Fi(c)2983 3068 y Fu(.)36 b(F)-7 b(rom)24 |
627423 |
> |
b(these)h(initial)h(results,)f(w)n(e)2042 3163 y(w)n(ould)g(not)h(b)r |
627424 |
|
(e)g(surprised)e(if)i(results)f(from)h(the)g(other)f(common)2042 |
627425 |
< |
4628 y(w)n(ater)35 b(mo)r(dels)i(sho)n(w)e(ice)i(0)f(to)g(b)r(e)h(the)g |
627426 |
< |
(lo)n(w)n(est)e(energy)g(crys-)2042 4724 y(tal)26 b(structure.)36 |
627425 |
> |
3259 y(w)n(ater)35 b(mo)r(dels)i(sho)n(w)e(ice)i(0)f(to)g(b)r(e)h(the)g |
627426 |
> |
(lo)n(w)n(est)e(energy)g(crys-)2042 3354 y(tal)26 b(structure.)36 |
627427 |
|
b(A)27 b(con)n(tin)n(uation)f(on)g(w)n(ork)f(studing)h(ice)h(0)f(with) |
627428 |
< |
2042 4819 y(m)n(ultip)r(oin)n(t)35 b(w)n(ater)f(mo)r(dels)h(will)g(b)r |
627429 |
< |
(e)g(published)g(in)g(a)g(coming)2042 4915 y(article.)p |
627430 |
< |
eop |
627428 |
> |
2042 3450 y(m)n(ultip)r(oin)n(t)35 b(w)n(ater)f(mo)r(dels)h(will)g(b)r |
627429 |
> |
(e)g(published)g(in)g(a)g(coming)2042 3545 y(article.)2631 |
627430 |
> |
3821 y Fo(IV.)88 b(CONCLUSIONS)2125 4035 y Fu(The)49 |
627431 |
> |
b(densit)n(y)g(maxim)n(um)f(and)h(temp)r(erature)g(dep)r(enden)n(t)2042 |
627432 |
> |
4130 y(transp)r(ort)25 b(for)h(the)g(SSD)h(w)n(ater)e(mo)r(del,)i(b)r |
627433 |
> |
(oth)f(with)h(and)f(with-)2042 4226 y(out)j(the)g(use)g(of)g(reaction)e |
627434 |
> |
(\014eld,)j(w)n(ere)e(studied)h(via)g(a)f(series)g(of)2042 |
627435 |
> |
4321 y(NPT)h(and)g(NVE)g(sim)n(ulations.)41 b(The)29 |
627436 |
> |
b(constan)n(t)g(pressure)e(sim-)2042 4417 y(ulations)34 |
627437 |
> |
b(of)h(the)h(melting)f(of)g(b)r(oth)g Fj(I)3264 4429 |
627438 |
> |
y Fi(h)3343 4417 y Fu(and)g Fj(I)3548 4429 y Fi(c)3617 |
627439 |
> |
4417 y Fu(ice)g(sho)n(w)n(ed)f(a)2042 4512 y(densit)n(y)c(maxim)n(um)f |
627440 |
> |
(near)h(260)e(K.)i(In)g(most)g(cases,)g(the)g(calcu-)2042 |
627441 |
> |
4608 y(lated)25 b(densities)f(w)n(ere)g(signi\014can)n(tly)g(lo)n(w)n |
627442 |
> |
(er)f(than)i(the)g(densities)2042 4703 y(calculated)k(in)h(sim)n |
627443 |
> |
(ulations)f(of)h(other)f(w)n(ater)g(mo)r(dels.)44 b(Analy-)2042 |
627444 |
> |
4799 y(sis)24 b(of)g(particle)f(di\013usion)i(sho)n(w)n(ed)e(SSD)i(to)f |
627445 |
> |
(capture)g(the)g(trans-)2042 4894 y(p)r(ort)d(prop)r(erties)f(of)i(exp) |
627446 |
> |
r(erimen)n(tal)f(v)n(ery)f(w)n(ell)h(in)h(b)r(oth)g(the)f(nor-)2042 |
627447 |
> |
4990 y(mal)27 b(and)h(sup)r(er-co)r(oled)e(liquid)i(regimes.)37 |
627448 |
> |
b(In)28 b(order)e(to)i(correct)2042 5085 y(the)35 b(densit)n(y)g(b)r |
627449 |
> |
(eha)n(vior,)h(SSD)g(w)n(as)e(reparameterized)g(for)g(use)2042 |
627450 |
> |
5180 y(b)r(oth)h(with)g(and)f(without)h(a)f(long-range)f(in)n |
627451 |
> |
(teraction)g(correc-)2042 5276 y(tion,)39 b(SSD/RF)e(and)f(SSD/E)g |
627452 |
> |
(resp)r(ectiv)n(ely)-7 b(.)63 b(In)37 b(addition)f(to)2042 |
627453 |
> |
5371 y(correcting)c(the)h(abnormally)g(lo)n(w)f(densities,)j(these)f |
627454 |
> |
(new)g(v)n(er-)p eop |
627455 |
|
%%Page: 11 11 |
627456 |
< |
11 10 bop 4001 -299 a Fu(11)439 -83 y Fo(IV.)88 b(CONCLUSIONS)-67 |
627457 |
< |
131 y Fu(The)49 b(densit)n(y)g(maxim)n(um)f(and)h(temp)r(erature)g(dep) |
627458 |
< |
r(enden)n(t)-150 226 y(transp)r(ort)25 b(for)h(the)g(SSD)h(w)n(ater)e |
627459 |
< |
(mo)r(del,)i(b)r(oth)g(with)f(and)g(with-)-150 322 y(out)j(the)g(use)g |
635838 |
< |
(of)g(reaction)f(\014eld,)h(w)n(ere)f(studied)i(via)e(a)h(series)e(of) |
635839 |
< |
-150 417 y(NPT)i(and)g(NVE)g(sim)n(ulations.)41 b(The)29 |
635840 |
< |
b(constan)n(t)g(pressure)f(sim-)-150 512 y(ulations)34 |
635841 |
< |
b(of)h(the)h(melting)f(of)g(b)r(oth)g Fj(I)1072 524 y |
635842 |
< |
Fi(h)1151 512 y Fu(and)g Fj(I)1356 524 y Fi(c)1425 512 |
635843 |
< |
y Fu(ice)g(sho)n(w)n(ed)f(a)-150 608 y(densit)n(y)c(maxim)n(um)g(near)f |
635844 |
< |
(260)f(K.)i(In)g(most)g(cases,)g(the)g(calcu-)-150 703 |
635845 |
< |
y(lated)25 b(densities)g(w)n(ere)e(signi\014can)n(tly)h(lo)n(w)n(er)f |
635846 |
< |
(than)i(the)g(densities)-150 799 y(calculated)k(in)h(sim)n(ulations)f |
635847 |
< |
(of)h(other)g(w)n(ater)e(mo)r(dels.)44 b(Analy-)-150 |
635848 |
< |
894 y(sis)24 b(of)g(particle)g(di\013usion)g(sho)n(w)n(ed)f(SSD)i(to)f |
635849 |
< |
(capture)g(the)g(trans-)-150 990 y(p)r(ort)d(prop)r(erties)g(of)g(exp)r |
635850 |
< |
(erimen)n(tal)g(v)n(ery)f(w)n(ell)h(in)h(b)r(oth)g(the)g(nor-)-150 |
635851 |
< |
1085 y(mal)28 b(and)f(sup)r(er-co)r(oled)g(liquid)h(regimes.)36 |
635852 |
< |
b(In)28 b(order)e(to)i(correct)-150 1181 y(the)36 b(densit)n(y)f(b)r |
635853 |
< |
(eha)n(vior,)h(SSD)f(w)n(as)g(reparameterized)e(for)i(use)-150 |
635854 |
< |
1276 y(b)r(oth)g(with)g(and)g(without)g(a)f(long-range)e(in)n |
635855 |
< |
(teraction)h(correc-)-150 1372 y(tion,)39 b(SSD/RF)e(and)f(SSD/E)h |
635856 |
< |
(resp)r(ectiv)n(ely)-7 b(.)62 b(In)37 b(addition)g(to)-150 |
635857 |
< |
1467 y(correcting)32 b(the)i(abnormally)e(lo)n(w)h(densities,)i(these)e |
635858 |
< |
(new)h(v)n(er-)-150 1563 y(sions)28 b(w)n(ere)f(sho)n(w)h(to)g(main)n |
635859 |
< |
(tain)g(or)g(impro)n(v)n(e)f(up)r(on)i(the)f(trans-)-150 |
635860 |
< |
1658 y(p)r(ort)f(and)f(structural)h(features)f(of)h(the)g(original)e(w) |
635861 |
< |
n(ater)h(mo)r(del,)-150 1754 y(all)19 b(while)h(main)n(taining)e(the)i |
627456 |
> |
11 10 bop 4001 -299 a Fu(11)-150 -83 y(sions)28 b(w)n(ere)f(sho)n(w)h |
627457 |
> |
(to)g(main)n(tain)g(or)g(impro)n(v)n(e)f(up)r(on)i(the)f(trans-)-150 |
627458 |
> |
12 y(p)r(ort)f(and)f(structural)h(features)f(of)h(the)g(original)e(w)n |
627459 |
> |
(ater)h(mo)r(del,)-150 108 y(all)19 b(while)h(main)n(taining)e(the)i |
627460 |
|
(fast)f(p)r(erformance)f(of)i(the)f(SSD)i(w)n(a-)-150 |
627461 |
< |
1849 y(ter)30 b(mo)r(del.)46 b(This)30 b(w)n(ork)f(sho)n(ws)g(these)i |
627462 |
< |
(simple)f(w)n(ater)f(mo)r(dels,)-150 1945 y(and)36 b(in)g(particular)f |
627461 |
> |
203 y(ter)30 b(mo)r(del.)46 b(This)30 b(w)n(ork)f(sho)n(ws)g(these)i |
627462 |
> |
(simple)f(w)n(ater)f(mo)r(dels,)-150 299 y(and)36 b(in)g(particular)f |
627463 |
|
(SSD/E)g(and)h(SSD/RF,)h(to)e(b)r(e)i(excellen)n(t)-150 |
627464 |
< |
2040 y(c)n(hoices)31 b(to)g(represen)n(t)g(explicit)h(w)n(ater)e(in)i |
627465 |
< |
(future)g(sim)n(ulations)-150 2136 y(of)c(bio)r(c)n(hemical)f(systems.) |
627466 |
< |
286 2412 y Fo(V.)87 b(A)n(CKNO)n(WLEDGMENTS)-67 2625 |
627467 |
< |
y Fu(The)29 b(authors)f(w)n(ould)g(lik)n(e)g(to)h(thank)g(the)g |
627468 |
< |
(National)f(Science)-150 2721 y(F)-7 b(oundation)21 b(for)f(funding)h |
627469 |
< |
(under)g(gran)n(t)e(CHE-0134881.)31 b(Com-)-150 2816 |
627470 |
< |
y(putation)19 b(time)h(w)n(as)e(pro)n(vided)g(b)n(y)g(the)i(Notre)e |
627471 |
< |
(Dame)h(Bunc)n(h-of-)-150 2912 y(Bo)n(xes)29 b(\(B.o.B\))i(computer)g |
627472 |
< |
(cluster)f(under)h(NSF)g(gran)n(t)f(DMR)-150 3007 y(00)d(79647.)570 |
627473 |
< |
3283 y Fo(REFERENCES)-117 3467 y Fn(1)-46 3497 y Fu(W.)39 |
627464 |
> |
394 y(c)n(hoices)31 b(to)g(represen)n(t)g(explicit)h(w)n(ater)e(in)i |
627465 |
> |
(future)g(sim)n(ulations)-150 490 y(of)c(bio)r(c)n(hemical)f(systems.) |
627466 |
> |
286 766 y Fo(V.)87 b(A)n(CKNO)n(WLEDGMENTS)-67 980 y |
627467 |
> |
Fu(Supp)r(ort)27 b(for)g(this)g(pro)5 b(ject)26 b(w)n(as)g(pro)n(vided) |
627468 |
> |
g(b)n(y)h(the)g(National)-150 1075 y(Science)i(F)-7 b(oundation)29 |
627469 |
> |
b(under)g(gran)n(t)e(CHE-0134881.)38 b(Compu-)-150 1171 |
627470 |
> |
y(tation)30 b(time)h(w)n(as)f(pro)n(vided)f(b)n(y)i(the)g(Notre)f(Dame) |
627471 |
> |
g(Bunc)n(h-of-)-150 1266 y(Bo)n(xes)f(\(B.o.B\))i(computer)g(cluster)f |
627472 |
> |
(under)h(NSF)g(gran)n(t)f(DMR)-150 1361 y(00)d(79647.)570 |
627473 |
> |
1638 y Fo(REFERENCES)-117 1821 y Fn(1)-46 1851 y Fu(W.)39 |
627474 |
|
b(L.)g(Jorgensen,)h(J.)f(Chandrasekhar,)h(J.)f(D.)g(Madura,)-46 |
627475 |
< |
3592 y(R.)c(W.)h(Imp)r(ey)-7 b(,)38 b(and)d(M.)g(L.)h(Klein,)h(J.)e |
627476 |
< |
(Chem.)g(Ph)n(ys.)g Fh(79)p Fu(,)-46 3688 y(926)26 b(\(1983\).)-117 |
627477 |
< |
3753 y Fn(2)-46 3783 y Fu(H.)62 b(J.)f(C.)h(Berendsen,)69 |
627475 |
> |
1947 y(R.)c(W.)h(Imp)r(ey)-7 b(,)38 b(and)d(M.)g(L.)h(Klein,)h(J.)e |
627476 |
> |
(Chem.)g(Ph)n(ys.)g Fh(79)p Fu(,)-46 2042 y(926)26 b(\(1983\).)-117 |
627477 |
> |
2107 y Fn(2)-46 2138 y Fu(H.)62 b(J.)f(C.)h(Berendsen,)69 |
627478 |
|
b(J.)62 b(R.)g(Grigera,)68 b(and)62 b(T.)g(P)-7 b(.)-46 |
627479 |
< |
3879 y(Straatsma,)26 b(J.)h(Ph)n(ys.)g(Chem.)h Fh(91)p |
627480 |
< |
Fu(,)f(6269)f(\(1987\).)-117 3944 y Fn(3)-46 3974 y Fu(M.)c(W.)h |
627479 |
> |
2233 y(Straatsma,)26 b(J.)h(Ph)n(ys.)g(Chem.)h Fh(91)p |
627480 |
> |
Fu(,)f(6269)f(\(1987\).)-117 2298 y Fn(3)-46 2329 y Fu(M.)c(W.)h |
627481 |
|
(Mahoney)e(and)h(W.)g(L.)h(Jorgensen,)e(J.)h(Chem.)g(Ph)n(ys.)-46 |
627482 |
< |
4070 y Fh(112)p Fu(\(20\),)k(8910)g(\(2000\).)-117 4135 |
627483 |
< |
y Fn(4)-46 4165 y Fu(M.)c(W.)h(Mahoney)e(and)h(W.)g(L.)h(Jorgensen,)e |
627484 |
< |
(J.)h(Chem.)g(Ph)n(ys.)-46 4261 y Fh(114)p Fu(\(1\),)27 |
627485 |
< |
b(363)f(\(2001\).)-117 4326 y Fn(5)-46 4356 y Fu(Y.)19 |
627482 |
> |
2424 y Fh(112)p Fu(\(20\),)k(8910)g(\(2000\).)-117 2489 |
627483 |
> |
y Fn(4)-46 2520 y Fu(M.)c(W.)h(Mahoney)e(and)h(W.)g(L.)h(Jorgensen,)e |
627484 |
> |
(J.)h(Chem.)g(Ph)n(ys.)-46 2615 y Fh(114)p Fu(\(1\),)27 |
627485 |
> |
b(363)f(\(2001\).)-117 2680 y Fn(5)-46 2710 y Fu(Y.)19 |
627486 |
|
b(Liu)g(and)g(T.)g(Ic)n(hiy)n(e,)h(J.)e(Ph)n(ys.)g(Chem.)i |
627487 |
< |
Fh(100)p Fu(,)g(2723)d(\(1996\).)-117 4422 y Fn(6)-46 |
627488 |
< |
4452 y Fu(D.)36 b(Bratk)n(o,)h(L.)f(Blum,)j(and)d(A.)h(Luzar,)h(J.)e |
627489 |
< |
(Chem.)g(Ph)n(ys.)-46 4547 y Fh(83)p Fu(\(12\),)26 b(6367)g(\(1985\).) |
627490 |
< |
2075 -113 y Fn(7)2145 -83 y Fu(L.)32 b(Blum,)i(F.)e(V)-7 |
627491 |
< |
b(ericat,)33 b(and)f(D.)h(Bratk)n(o,)e(J.)h(Chem.)g(Ph)n(ys.)2145 |
627492 |
< |
12 y Fh(102)p Fu(\(3\),)27 b(1461)f(\(1995\).)2075 78 |
627493 |
< |
y Fn(8)2145 108 y Fu(A.)40 b(Chandra)d(and)i(T.)g(Ic)n(hiy)n(e,)i(J.)e |
627494 |
< |
(Chem.)g(Ph)n(ys.)f Fh(111)p Fu(\(6\),)2145 203 y(2701)26 |
627495 |
< |
b(\(1999\).)2075 269 y Fn(9)2145 299 y Fu(C.)46 b(Sagui)e(and)h(T.)g |
627496 |
< |
(A.)h(Darden,)j(Ann)n(u.)d(Rev.)f(Bioph)n(ys.)2145 394 |
627497 |
< |
y(Biomol.)27 b(Struct.)h Fh(28)p Fu(,)f(155)g(\(1999\).)2042 |
627498 |
< |
460 y Fn(10)2145 490 y Fu(M.-L.)k(T)-7 b(an,)31 b(J.)f(T.)g(Fisc)n |
627499 |
< |
(her,)h(A.)g(Chandra,)f(B.)g(R.)h(Bro)r(oks,)2145 585 |
627500 |
< |
y(and)d(T.)f(Ic)n(hiy)n(e,)g(Chem.)h(Ph)n(ys.)f(Lett.)h |
627501 |
< |
Fh(376)p Fu(,)f(646)f(\(2003\).)2042 651 y Fn(11)2145 |
627502 |
< |
681 y Fu(M.)f(P)-7 b(.)24 b(Allen)h(and)g(D.)g(J.)f(Tildesley)-7 |
627503 |
< |
b(,)25 b Fm(Computer)j(Simulation)2145 776 y(of)d(Liquids)k |
627487 |
> |
Fh(100)p Fu(,)g(2723)d(\(1996\).)-117 2776 y Fn(6)-46 |
627488 |
> |
2806 y Fu(D.)36 b(Bratk)n(o,)h(L.)f(Blum,)j(and)d(A.)h(Luzar,)h(J.)e |
627489 |
> |
(Chem.)g(Ph)n(ys.)-46 2901 y Fh(83)p Fu(\(12\),)26 b(6367)g(\(1985\).) |
627490 |
> |
-117 2967 y Fn(7)-46 2997 y Fu(L.)32 b(Blum,)h(F.)f(V)-7 |
627491 |
> |
b(ericat,)33 b(and)f(D.)h(Bratk)n(o,)e(J.)h(Chem.)g(Ph)n(ys.)-46 |
627492 |
> |
3092 y Fh(102)p Fu(\(3\),)27 b(1461)e(\(1995\).)-117 |
627493 |
> |
3158 y Fn(8)-46 3188 y Fu(A.)39 b(Chandra)f(and)g(T.)h(Ic)n(hiy)n(e,)i |
627494 |
> |
(J.)e(Chem.)g(Ph)n(ys.)f Fh(111)p Fu(\(6\),)-46 3283 |
627495 |
> |
y(2701)25 b(\(1999\).)-117 3349 y Fn(9)-46 3379 y Fu(C.)45 |
627496 |
> |
b(Sagui)f(and)h(T.)h(A.)f(Darden,)50 b(Ann)n(u.)45 b(Rev.)g(Bioph)n |
627497 |
> |
(ys.)-46 3474 y(Biomol.)26 b(Struct.)i Fh(28)p Fu(,)g(155)e(\(1999\).) |
627498 |
> |
-150 3540 y Fn(10)-46 3570 y Fu(M.-L.)k(T)-7 b(an,)31 |
627499 |
> |
b(J.)f(T.)h(Fisc)n(her,)f(A.)h(Chandra,)f(B.)g(R.)h(Bro)r(oks,)-46 |
627500 |
> |
3665 y(and)c(T.)h(Ic)n(hiy)n(e,)f(Chem.)g(Ph)n(ys.)g(Lett.)h |
627501 |
> |
Fh(376)p Fu(,)f(646)f(\(2003\).)2042 -113 y Fn(11)2145 |
627502 |
> |
-83 y Fu(M.)f(P)-7 b(.)24 b(Allen)h(and)g(D.)g(J.)f(Tildesley)-7 |
627503 |
> |
b(,)25 b Fm(Computer)j(Simulation)2145 12 y(of)d(Liquids)k |
627504 |
|
Fu(\(Oxford)20 b(Univ)n(ersit)n(y)g(Press,)h(New)g(Y)-7 |
627505 |
< |
b(ork,)22 b(1987\).)2042 842 y Fn(12)2145 872 y Fu(D.)42 |
627505 |
> |
b(ork,)22 b(1987\).)2042 78 y Fn(12)2145 108 y Fu(D.)42 |
627506 |
|
b(v)-5 b(an)41 b(der)f(Sp)r(o)r(el,)45 b(P)-7 b(.)41 |
627507 |
|
b(J.)f(v)-5 b(an)41 b(Maaren,)i(and)e(H.)g(J.)g(C.)2145 |
627508 |
< |
967 y(Berendsen,)27 b(J.)h(Chem.)g(Ph)n(ys.)e Fh(111)p |
627509 |
< |
Fu(\(6\),)h(10220)e(\(1998\).)2042 1033 y Fn(13)2145 |
627510 |
< |
1063 y Fu(W.)j(G.)g(Ho)r(o)n(v)n(er,)e(Ph)n(ys.)h(Rev.)g(A)h |
627511 |
< |
Fh(31)p Fu(\(3\),)g(1695)d(\(1985\).)2042 1128 y Fn(14)2145 |
627512 |
< |
1158 y Fu(W.)j(G.)g(Ho)r(o)n(v)n(er,)e(Ph)n(ys.)h(Rev.)g(A)h |
627513 |
< |
Fh(34)p Fu(\(3\),)g(2499)d(\(1986\).)2042 1224 y Fn(15)2145 |
627514 |
< |
1254 y Fu(A.)35 b(Dullw)n(eb)r(er,)h(B.)d(Leimkuhler,)j(and)e(R.)g |
627515 |
< |
(McLac)n(hlan,)g(J.)2145 1349 y(Chem.)28 b(Ph)n(ys.)f |
627516 |
< |
Fh(107)p Fu(\(15\),)f(5840)g(\(1997\).)2042 1414 y Fn(16)2145 |
627517 |
< |
1445 y Fu(A.)31 b(Kol,)f(B.)g(B.)g(Laird,)g(and)g(B.)g(J.)g |
627518 |
< |
(Leimkuhler,)h(J.)f(Chem.)2145 1540 y(Ph)n(ys.)d Fh(107)p |
627519 |
< |
Fu(\(7\),)g(2580)f(\(1997\).)2042 1605 y Fn(17)2145 1636 |
627520 |
< |
y Fu(J.)g(D.)g(Bernal)f(and)h(R.)g(H.)g(F)-7 b(o)n(wler,)26 |
627521 |
< |
b(J.)f(Chem.)i(Ph)n(ys.)d Fh(1)p Fu(,)j(515)2145 1731 |
627522 |
< |
y(\(1933\).)2042 1796 y Fn(18)2145 1826 y Fu(A.)20 b(Rahman)f(and)g(F.) |
627523 |
< |
g(H.)h(Stillinger,)h(J.)e(Chem.)g(Ph)n(ys.)g Fh(57)p |
627524 |
< |
Fu(\(9\),)2145 1922 y(4009)26 b(\(1972\).)2042 1987 y |
627525 |
< |
Fn(19)2145 2017 y Fu(W.)37 b(L.)f(Jorgensen)f(and)h(C.)g(Jenson,)i(J.)e |
627526 |
< |
(Comput.)h(Chem.)2145 2113 y Fh(19)p Fu(\(10\),)27 b(1179)f(\(1998\).) |
627527 |
< |
2042 2178 y Fn(20)2145 2208 y Fu(L.)35 b(A.)g(B\023)-42 |
627528 |
< |
b(aez)34 b(and)h(P)-7 b(.)35 b(Clancy)-7 b(,)36 b(J.)e(Chem.)h(Ph)n |
627529 |
< |
(ys.)f Fh(101)p Fu(\(11\),)2145 2304 y(9837)26 b(\(1994\).)2042 |
627530 |
< |
2369 y Fn(21)2145 2399 y Fu(R.)37 b(C.)g(W)-7 b(east,)39 |
627531 |
< |
b(ed.,)h Fm(CR)n(C)e(Handb)l(o)l(ok)h(of)g(Chemistry)h(and)2145 |
627532 |
< |
2495 y(Physics)50 b Fu(\(CR)n(C)41 b(Press,)j(Inc.,)h(Bo)r(ca)40 |
627533 |
< |
b(Raton,)k(FL,)e(1980\),)2145 2590 y(60th)27 b(ed.)2042 |
627534 |
< |
2656 y Fn(22)2145 2686 y Fu(Gillen,)33 b(Douglas,)f(and)f(Ho)r(c)n(h,)h |
627535 |
< |
(J.)g(Chem.)g(Ph)n(ys.)e Fh(57)p Fu(,)i(5117)2145 2781 |
627536 |
< |
y(\(1972\).)2042 2847 y Fn(23)2145 2877 y Fu(R.)c(Mills,)g(J.)f(Ph)n |
627537 |
< |
(ys.)g(Chem.)h Fh(77)p Fu(\(5\),)f(685)f(\(1973\).)2042 |
627538 |
< |
2942 y Fn(24)2145 2972 y Fu(G.)d(Hura,)g(J.)f(M.)h(Sorenson,)f(R.)g(M.) |
627539 |
< |
h(Glaeser,)f(and)g(T.)h(Head-)2145 3068 y(Gordon,)k(J.)g(Chem.)h(Ph)n |
627540 |
< |
(ys.)f Fh(113)p Fu(\(20\),)f(9140)g(\(2000\).)2042 3133 |
627541 |
< |
y Fn(25)2145 3163 y Fu(A.)h(K.)e(Sop)r(er)h(and)g(M.)g(G.)g(Phillips,)g |
627542 |
< |
(Chem.)h(Ph)n(ys.)e Fh(107)p Fu(\(1\),)2145 3259 y(47)i(\(1986\).)2042 |
627543 |
< |
3324 y Fn(26)2145 3354 y Fu(M.)h(Sprik,)g(J.)f(Chem.)h(Ph)n(ys.)e |
627544 |
< |
Fh(95)p Fu(\(9\),)i(6762)d(\(1991\).)2042 3419 y Fn(27)2145 |
627545 |
< |
3450 y Fu(A.)36 b(V.)g(Gubsk)-5 b(a)n(y)n(a)35 b(and)g(P)-7 |
627546 |
< |
b(.)35 b(G.)h(Kusalik,)h(J.)e(Chem.)h(Ph)n(ys.)2145 3545 |
627547 |
< |
y Fh(117)p Fu(\(11\),)27 b(5290)f(\(2002\).)2042 3610 |
627548 |
< |
y Fn(28)2145 3641 y Fu(Y.)e(S.)f(Bady)n(al,)g(M.)g(L.)g(Sab)r(oungi,)g |
627549 |
< |
(D.)h(L.)f(Price,)g(S.)g(D.)h(Shas-)2145 3736 y(tri,)30 |
627508 |
> |
203 y(Berendsen,)27 b(J.)h(Chem.)g(Ph)n(ys.)e Fh(111)p |
627509 |
> |
Fu(\(6\),)h(10220)e(\(1998\).)2042 269 y Fn(13)2145 299 |
627510 |
> |
y Fu(W.)j(G.)g(Ho)r(o)n(v)n(er,)e(Ph)n(ys.)h(Rev.)g(A)h |
627511 |
> |
Fh(31)p Fu(\(3\),)g(1695)d(\(1985\).)2042 364 y Fn(14)2145 |
627512 |
> |
394 y Fu(W.)j(G.)g(Ho)r(o)n(v)n(er,)e(Ph)n(ys.)h(Rev.)g(A)h |
627513 |
> |
Fh(34)p Fu(\(3\),)g(2499)d(\(1986\).)2042 460 y Fn(15)2145 |
627514 |
> |
490 y Fu(A.)35 b(Dullw)n(eb)r(er,)h(B.)d(Leimkuhler,)j(and)e(R.)g |
627515 |
> |
(McLac)n(hlan,)g(J.)2145 585 y(Chem.)28 b(Ph)n(ys.)f |
627516 |
> |
Fh(107)p Fu(\(15\),)f(5840)g(\(1997\).)2042 651 y Fn(16)2145 |
627517 |
> |
681 y Fu(A.)31 b(Kol,)f(B.)g(B.)g(Laird,)g(and)g(B.)g(J.)g(Leimkuhler,) |
627518 |
> |
h(J.)f(Chem.)2145 776 y(Ph)n(ys.)d Fh(107)p Fu(\(7\),)g(2580)f |
627519 |
> |
(\(1997\).)2042 842 y Fn(17)2145 872 y Fu(J.)g(D.)g(Bernal)f(and)h(R.)g |
627520 |
> |
(H.)g(F)-7 b(o)n(wler,)26 b(J.)f(Chem.)i(Ph)n(ys.)d Fh(1)p |
627521 |
> |
Fu(,)j(515)2145 967 y(\(1933\).)2042 1033 y Fn(18)2145 |
627522 |
> |
1063 y Fu(A.)20 b(Rahman)f(and)g(F.)g(H.)h(Stillinger,)h(J.)e(Chem.)g |
627523 |
> |
(Ph)n(ys.)g Fh(57)p Fu(\(9\),)2145 1158 y(4009)26 b(\(1972\).)2042 |
627524 |
> |
1224 y Fn(19)2145 1254 y Fu(W.)37 b(L.)f(Jorgensen)f(and)h(C.)g |
627525 |
> |
(Jenson,)i(J.)e(Comput.)h(Chem.)2145 1349 y Fh(19)p Fu(\(10\),)27 |
627526 |
> |
b(1179)f(\(1998\).)2042 1414 y Fn(20)2145 1445 y Fu(L.)35 |
627527 |
> |
b(A.)g(B\023)-42 b(aez)34 b(and)h(P)-7 b(.)35 b(Clancy)-7 |
627528 |
> |
b(,)36 b(J.)e(Chem.)h(Ph)n(ys.)f Fh(101)p Fu(\(11\),)2145 |
627529 |
> |
1540 y(9837)26 b(\(1994\).)2042 1605 y Fn(21)2145 1636 |
627530 |
> |
y Fu(R.)37 b(C.)g(W)-7 b(east,)39 b(ed.,)h Fm(CR)n(C)e(Handb)l(o)l(ok)h |
627531 |
> |
(of)g(Chemistry)h(and)2145 1731 y(Physics)50 b Fu(\(CR)n(C)41 |
627532 |
> |
b(Press,)j(Inc.,)h(Bo)r(ca)40 b(Raton,)k(FL,)e(1980\),)2145 |
627533 |
> |
1826 y(60th)27 b(ed.)2042 1892 y Fn(22)2145 1922 y Fu(Gillen,)33 |
627534 |
> |
b(Douglas,)f(and)f(Ho)r(c)n(h,)h(J.)g(Chem.)g(Ph)n(ys.)e |
627535 |
> |
Fh(57)p Fu(,)i(5117)2145 2017 y(\(1972\).)2042 2083 y |
627536 |
> |
Fn(23)2145 2113 y Fu(R.)c(Mills,)g(J.)f(Ph)n(ys.)g(Chem.)h |
627537 |
> |
Fh(77)p Fu(\(5\),)f(685)f(\(1973\).)2042 2178 y Fn(24)2145 |
627538 |
> |
2208 y Fu(G.)d(Hura,)g(J.)f(M.)h(Sorenson,)f(R.)g(M.)h(Glaeser,)f(and)g |
627539 |
> |
(T.)h(Head-)2145 2304 y(Gordon,)k(J.)g(Chem.)h(Ph)n(ys.)f |
627540 |
> |
Fh(113)p Fu(\(20\),)f(9140)g(\(2000\).)2042 2369 y Fn(25)2145 |
627541 |
> |
2399 y Fu(A.)h(K.)e(Sop)r(er)h(and)g(M.)g(G.)g(Phillips,)g(Chem.)h(Ph)n |
627542 |
> |
(ys.)e Fh(107)p Fu(\(1\),)2145 2495 y(47)i(\(1986\).)2042 |
627543 |
> |
2560 y Fn(26)2145 2590 y Fu(M.)h(Sprik,)g(J.)f(Chem.)h(Ph)n(ys.)e |
627544 |
> |
Fh(95)p Fu(\(9\),)i(6762)d(\(1991\).)2042 2656 y Fn(27)2145 |
627545 |
> |
2686 y Fu(A.)36 b(V.)g(Gubsk)-5 b(a)n(y)n(a)35 b(and)g(P)-7 |
627546 |
> |
b(.)35 b(G.)h(Kusalik,)h(J.)e(Chem.)h(Ph)n(ys.)2145 2781 |
627547 |
> |
y Fh(117)p Fu(\(11\),)27 b(5290)f(\(2002\).)2042 2847 |
627548 |
> |
y Fn(28)2145 2877 y Fu(Y.)e(S.)f(Bady)n(al,)g(M.)g(L.)g(Sab)r(oungi,)g |
627549 |
> |
(D.)h(L.)f(Price,)g(S.)g(D.)h(Shas-)2145 2972 y(tri,)30 |
627550 |
|
b(D.)g(R.)f(Hae\013ner,)g(and)g(A.)h(K.)f(Sop)r(er,)g(J.)g(Chem.)g(Ph)n |
627551 |
< |
(ys.)2145 3831 y Fh(112)p Fu(\(21\),)e(9206)f(\(2000\).)2042 |
627552 |
< |
3897 y Fn(29)2145 3927 y Fu(J.)c(Barriol)d(and)j(A.)g(W)-7 |
627551 |
> |
(ys.)2145 3068 y Fh(112)p Fu(\(21\),)e(9206)f(\(2000\).)2042 |
627552 |
> |
3133 y Fn(29)2145 3163 y Fu(J.)c(Barriol)d(and)j(A.)g(W)-7 |
627553 |
|
b(eisb)r(ec)n(k)n(er,)22 b(Compt.)g(Rend.)g(Acad.)f(Sc.)2145 |
627554 |
< |
4022 y(P)n(aris)26 b Fh(259)p Fu(,)h(4643)f(\(1964\).)2042 |
627555 |
< |
4088 y Fn(30)2145 4118 y Fu(B.)32 b(R.)g(Bro)r(oks,)g(R.)g(E.)f |
627556 |
< |
(Bruccoleri,)h(B.)g(D.)g(Olafson,)g(D.)g(J.)2145 4213 |
627554 |
> |
3259 y(P)n(aris)26 b Fh(259)p Fu(,)h(4643)f(\(1964\).)2042 |
627555 |
> |
3324 y Fn(30)2145 3354 y Fu(B.)32 b(R.)g(Bro)r(oks,)g(R.)g(E.)f |
627556 |
> |
(Bruccoleri,)h(B.)g(D.)g(Olafson,)g(D.)g(J.)2145 3450 |
627557 |
|
y(States,)27 b(S.)f(Sw)n(aminathan,)g(and)g(M.)g(Karplus,)f(J.)h |
627558 |
< |
(Comput.)2145 4309 y(Chem.)i Fh(4)p Fu(\(2\),)g(187)e(\(1983\).)p |
627558 |
> |
(Comput.)2145 3545 y(Chem.)i Fh(4)p Fu(\(2\),)g(187)e(\(1983\).)p |
627559 |
|
eop |
627560 |
|
%%Trailer |
627561 |
|
end |