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Revision 743 by chrisfen, Wed Sep 3 21:36:09 2003 UTC vs.
Revision 757 by chrisfen, Wed Sep 10 15:38:43 2003 UTC

# Line 10 | Line 10
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1337 < (melting)h(of)g(b)r(oth)379 1245 y Fp(I)413 1254 y Fo(h)472
1338 < 1245 y Fq(and)19 b Fp(I)649 1253 y Fo(c)700 1245 y Fq(ice)h(sho)n(w)n
1323 > 1 0 bop -113 36 a Fv(On)38 b(the)g(temp)s(erature)f(dep)s(enden)m(t)h
1324 > (structural)f(and)h(transp)s(ort)f(prop)s(erties)g(of)h(the)f(soft)h
1325 > (stic)m(ky)707 152 y(dip)s(ole)e(\(SSD\))h(and)i(related)e(single)f(p)s
1326 > (oin)m(t)h(w)m(ater)g(mo)s(dels)1060 488 y Fu(Christopher)j(J.)h(F)-7
1327 > b(ennell)41 b(and)g(J.)f(Daniel)h(Gezelter)2836 458 y
1328 > Ft(\003)1210 592 y Fs(Dep)l(artment)h(of)e(Chemistry)h(and)g(Bio)l
1329 > (chemistry)1509 679 y(University)j(of)f(Notr)l(e)h(Dame)1473
1330 > 767 y(Notr)l(e)g(Dame,)i(Indiana)c(46556)1460 905 y Fu(\(Dated:)c
1331 > (Septem)n(b)r(er)27 b(9,)h(2003\))456 977 y Fr(NVE)i(and)f(NPT)i
1332 > (molecular)f(dynamics)f(sim)n(ulations)i(w)n(ere)g(p)r(erformed)f(in)g
1333 > (order)g(to)g(in)n(v)n(estigate)h(the)379 1065 y(densit)n(y)e(maxim)n
1334 > (um)d(and)i(temp)r(erature)h(dep)r(enden)n(t)e(transp)r(ort)j(for)g
1335 > (the)f(SSD)f(w)n(ater)i(mo)r(del,)g(b)r(oth)f(with)379
1336 > 1152 y(and)c(without)f(the)h(use)f(of)i(reaction)f(\014eld.)34
1337 > b(The)25 b(constan)n(t)g(pressure)g(sim)n(ulations)g(of)g(the)f
1338 > (melting)h(of)g(b)r(oth)379 1239 y Fq(I)413 1248 y Fp(h)472
1339 > 1239 y Fr(and)19 b Fq(I)649 1247 y Fp(c)700 1239 y Fr(ice)h(sho)n(w)n
1340   (ed)f(a)h(densit)n(y)f(maxim)n(um)d(near)j(260)h(K.)g(In)e(most)h
1341   (cases,)j(the)d(calculated)h(densities)g(w)n(ere)379
1342 < 1332 y(signi\014can)n(tly)26 b(lo)n(w)n(er)h(than)e(the)g(densities)h
1342 > 1326 y(signi\014can)n(tly)26 b(lo)n(w)n(er)h(than)e(the)g(densities)h
1343   (calculated)g(in)f(sim)n(ulations)h(of)g(other)g(w)n(ater)g(mo)r(dels.)
1344 < 34 b(Analysis)379 1419 y(of)28 b(particle)g(di\013usion)f(sho)n(w)n(ed)
1344 > 34 b(Analysis)379 1413 y(of)28 b(particle)g(di\013usion)f(sho)n(w)n(ed)
1345   g(SSD)f(to)h(capture)g(the)f(transp)r(ort)h(prop)r(erties)h(of)g(exp)r
1346 < (erimen)n(tal)e(v)n(ery)g(w)n(ell)379 1506 y(in)i(b)r(oth)g(the)g
1346 > (erimen)n(tal)e(v)n(ery)g(w)n(ell)379 1501 y(in)i(b)r(oth)g(the)g
1347   (normal)g(and)g(sup)r(er-co)r(oled)h(liquid)f(regimes.)43
1348   b(In)27 b(order)i(to)f(correct)h(the)f(densit)n(y)f(b)r(eha)n(vior,)379
1349 < 1593 y(SSD)k(w)n(as)i(reparameterized)e(for)i(use)f(b)r(oth)f(with)h
1349 > 1588 y(SSD)k(w)n(as)i(reparameterized)e(for)i(use)f(b)r(oth)f(with)h
1350   (and)f(without)h(a)g(long-range)h(in)n(teraction)f(correction,)379
1351 < 1680 y(SSD/RF)23 b(and)g(SSD/E)h(resp)r(ectiv)n(ely)-6
1351 > 1675 y(SSD/RF)23 b(and)g(SSD/E)h(resp)r(ectiv)n(ely)-6
1352   b(.)33 b(In)23 b(addition)h(to)g(correcting)h(the)e(abnormally)h(lo)n
1353 < (w)h(densities,)g(these)379 1768 y(new)k(v)n(ersions)f(w)n(ere)h(sho)n
1353 > (w)h(densities,)g(these)379 1762 y(new)k(v)n(ersions)f(w)n(ere)h(sho)n
1354   (w)g(to)f(main)n(tain)g(or)h(impro)n(v)n(e)e(up)r(on)g(the)h(transp)r
1355 < (ort)h(and)e(structural)i(features)g(of)379 1855 y(the)d(original)h(w)n
1356 < (ater)f(mo)r(del.)436 2156 y Fn(I.)88 b(INTR)n(ODUCTION)-67
1357 < 2369 y Ft(One)24 b(of)h(the)g(most)f(imp)r(ortan)n(t)h(tasks)f(in)h
1358 < (sim)n(ulations)e(of)i(bio-)-150 2465 y(c)n(hemical)38
1355 > (ort)h(and)e(structural)i(features)g(of)379 1849 y(the)d(original)h(w)n
1356 > (ater)f(mo)r(del.)436 2150 y Fo(I.)88 b(INTR)n(ODUCTION)-67
1357 > 2364 y Fu(One)24 b(of)h(the)g(most)f(imp)r(ortan)n(t)h(tasks)f(in)h
1358 > (sim)n(ulations)e(of)i(bio-)-150 2459 y(c)n(hemical)38
1359   b(systems)g(is)g(the)h(prop)r(er)e(depiction)i(of)f(w)n(ater)g(and)-150
1360 < 2560 y(w)n(ater)24 b(solv)-5 b(ation.)35 b(In)25 b(fact,)g(the)g(bulk)g
1361 < (of)g(the)g(calculations)f(p)r(er-)-150 2656 y(formed)e(in)i(solv)-5
1360 > 2555 y(w)n(ater)24 b(solv)-5 b(ation.)35 b(In)25 b(fact,)g(the)g(bulk)g
1361 > (of)g(the)g(calculations)f(p)r(er-)-150 2650 y(formed)e(in)i(solv)-5
1362   b(ated)22 b(sim)n(ulations)g(are)g(of)g(in)n(teractions)g(with)h(or)
1363 < -150 2751 y(b)r(et)n(w)n(een)29 b(solv)n(en)n(t)f(molecules.)42
1364 < b(Th)n(us,)29 b(the)h(outcomes)e(of)h(these)-150 2847
1363 > -150 2746 y(b)r(et)n(w)n(een)29 b(solv)n(en)n(t)f(molecules.)42
1364 > b(Th)n(us,)29 b(the)h(outcomes)e(of)h(these)-150 2841
1365   y(t)n(yp)r(es)i(of)f(sim)n(ulations)g(are)g(highly)g(dep)r(enden)n(t)i
1366 < (on)e(the)h(ph)n(ysi-)-150 2942 y(cal)25 b(prop)r(erties)f(of)h(w)n
1366 > (on)e(the)h(ph)n(ysi-)-150 2937 y(cal)25 b(prop)r(erties)f(of)h(w)n
1367   (ater,)g(b)r(oth)g(as)g(individual)g(molecules)g(and)-150
1368 < 3038 y(in)42 b(groups/bulk.)76 b(Due)42 b(to)f(the)h(fact)f(that)h
1369 < (explicit)g(solv)n(en)n(t)-150 3133 y(accoun)n(ts)22
1368 > 3032 y(in)42 b(groups/bulk.)76 b(Due)42 b(to)f(the)h(fact)f(that)h
1369 > (explicit)g(solv)n(en)n(t)-150 3128 y(accoun)n(ts)22
1370   b(for)h(a)h(massiv)n(e)e(p)r(ortion)h(of)h(the)f(calculations,)h(it)g
1371 < (nec-)-150 3229 y(essary)38 b(to)h(simplify)h(the)g(solv)n(en)n(t)e(to)
1372 < i(some)f(exten)n(t)g(in)h(order)-150 3324 y(to)27 b(complete)h(sim)n
1371 > (nec-)-150 3223 y(essary)38 b(to)h(simplify)h(the)g(solv)n(en)n(t)e(to)
1372 > i(some)f(exten)n(t)g(in)h(order)-150 3318 y(to)27 b(complete)h(sim)n
1373   (ulations)f(in)h(a)f(reasonable)e(amoun)n(t)i(of)h(time.)-150
1374 < 3420 y(In)h(the)f(case)g(of)g(sim)n(ulating)g(w)n(ater)f(in)i
1375 < (bio-molecular)d(studies,)-150 3515 y(the)37 b(balance)f(b)r(et)n(w)n
1374 > 3414 y(In)h(the)f(case)g(of)g(sim)n(ulating)g(w)n(ater)f(in)i
1375 > (bio-molecular)d(studies,)-150 3509 y(the)37 b(balance)f(b)r(et)n(w)n
1376   (een)g(accurate)f(prop)r(erties)h(and)g(computa-)-150
1377 < 3610 y(tional)25 b(e\016ciency)h(is)g(esp)r(ecially)f(delicate,)h(and)f
1378 < (it)h(has)g(resulted)-150 3706 y(in)31 b(a)g(v)-5 b(ariet)n(y)31
1379 < b(of)g(di\013eren)n(t)g(w)n(ater)f(mo)r(dels.)1238 3676
1380 < y Fm(1{3)1373 3706 y Ft(Man)n(y)g(of)h(these)-150 3801
1377 > 3605 y(tional)25 b(e\016ciency)h(is)g(esp)r(ecially)f(delicate,)h(and)f
1378 > (it)h(has)g(resulted)-150 3700 y(in)31 b(a)g(v)-5 b(ariet)n(y)31
1379 > b(of)g(di\013eren)n(t)g(w)n(ater)f(mo)r(dels.)1238 3670
1380 > y Fn(1{3)1373 3700 y Fu(Man)n(y)g(of)h(these)-150 3796
1381   y(mo)r(dels)22 b(get)g(sp)r(eci\014c)g(prop)r(erties)f(correct)f(or)h
1382 < (b)r(etter)h(than)g(their)-150 3897 y(predecessors,)38
1382 > (b)r(etter)h(than)g(their)-150 3891 y(predecessors,)38
1383   b(but)h(this)f(is)g(often)g(at)g(a)f(cost)h(of)g(some)f(other)-150
1384 < 3992 y(prop)r(erties)g(or)g(of)g(computer)g(time.)68
1385 < b(As)38 b(an)f(example,)j(com-)-150 4088 y(pare)27 b(TIP3P)f(or)h
1384 > 3987 y(prop)r(erties)g(or)g(of)g(computer)g(time.)68
1385 > b(As)38 b(an)f(example,)j(com-)-150 4082 y(pare)27 b(TIP3P)f(or)h
1386   (TIP4P)f(to)h(TIP5P)-7 b(.)26 b(TIP5P)h(succeeds)g(in)g(im-)-150
1387 < 4183 y(pro)n(ving)j(the)j(structural)e(and)g(transp)r(ort)g(prop)r
1388 < (erties)g(o)n(v)n(er)f(its)-150 4279 y(predecessors,)36
1387 > 4178 y(pro)n(ving)j(the)j(structural)e(and)g(transp)r(ort)g(prop)r
1388 > (erties)g(o)n(v)n(er)f(its)-150 4273 y(predecessors,)36
1389   b(y)n(et)g(this)g(comes)g(at)g(a)f(greater)g(than)h(50\045)f(in-)-150
1390 < 4374 y(crease)30 b(in)h(computational)g(cost.)919 4344
1391 < y Fm(3)o(,4)1039 4374 y Ft(One)f(recen)n(tly)h(dev)n(elop)r(ed)-150
1392 < 4470 y(mo)r(del)36 b(that)g(succeeds)f(in)g(b)r(oth)h(retaining)f
1393 < (accuracy)f(of)h(sys-)-150 4565 y(tem)j(prop)r(erties)e(and)i
1394 < (simplifying)f(calculations)f(to)i(increase)-150 4661
1390 > 4369 y(crease)30 b(in)h(computational)g(cost.)919 4339
1391 > y Fn(3)o(,4)1039 4369 y Fu(One)f(recen)n(tly)h(dev)n(elop)r(ed)-150
1392 > 4464 y(mo)r(del)36 b(that)g(succeeds)f(in)g(b)r(oth)h(retaining)f
1393 > (accuracy)f(of)h(sys-)-150 4560 y(tem)j(prop)r(erties)e(and)i
1394 > (simplifying)f(calculations)f(to)i(increase)-150 4655
1395   y(computational)30 b(e\016ciency)g(is)h(the)f(Soft)h(Stic)n(ky)g(Dip)r
1396 < (ole)f(w)n(ater)-150 4756 y(mo)r(del.)92 4726 y Fm(5)-67
1397 < 4852 y Ft(The)e(Soft)h(Stic)n(ky)f(Dip)r(ole)h(\(SSD\))g(w)n(ater)f(mo)
1398 < 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
1399 < (e)e Fl(et)j(al.)67 b Ft(as)37 b(a)g(mo)r(di\014ed)h(form)f(of)h(the)f
1400 < (hard-)-150 5043 y(sphere)48 b(w)n(ater)g(mo)r(del)h(prop)r(osed)e(b)n
1401 < (y)i(Bratk)n(o,)j(Blum,)j(and)p -150 5212 300 4 v -59
1402 < 5390 a Fk(\003)-23 5413 y Fj(Corresp)r(onding)24 b(author.)55
1403 < b(Electronic)25 b(mail:)k(gezelter@nd.edu)2042 2156 y
1404 < Ft(Luzar.)2275 2126 y Fm(6)o(,7)2403 2156 y Ft(SSD)42
1396 > (ole)f(w)n(ater)-150 4751 y(mo)r(del.)92 4720 y Fn(5)-67
1397 > 4846 y Fu(The)e(Soft)h(Stic)n(ky)f(Dip)r(ole)h(\(SSD\))g(w)n(ater)f(mo)
1398 > 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
1399 > (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
1400 > (hard-)-150 5037 y(sphere)48 b(w)n(ater)g(mo)r(del)h(prop)r(osed)e(b)n
1401 > (y)i(Bratk)n(o,)j(Blum,)j(and)p -150 5206 300 4 v -59
1402 > 5384 a Fl(\003)-23 5407 y Fk(Corresp)r(onding)24 b(author.)55
1403 > b(Electronic)25 b(mail:)k(gezelter@nd.edu)2042 2150 y
1404 > Fu(Luzar.)2275 2120 y Fn(6)o(,7)2403 2150 y Fu(SSD)42
1405   b(consists)d(of)i(a)f(single)f(p)r(oin)n(t)i(dip)r(ole)g(with)g(a)2042
1406 < 2251 y(Lennard-Jones)35 b(core)i(and)h(a)f(stic)n(ky)g(p)r(oten)n(tial)
1407 < h(that)g(directs)2042 2347 y(the)27 b(particles)f(to)g(assume)g(the)h
1408 < (prop)r(er)e(h)n(ydrogen)g(b)r(ond)i(orien-)2042 2442
1406 > 2246 y(Lennard-Jones)35 b(core)i(and)h(a)f(stic)n(ky)g(p)r(oten)n(tial)
1407 > h(that)g(directs)2042 2341 y(the)27 b(particles)f(to)g(assume)g(the)h
1408 > (prop)r(er)e(h)n(ydrogen)g(b)r(ond)i(orien-)2042 2437
1409   y(tation)32 b(in)h(the)g(\014rst)f(solv)-5 b(ation)31
1410   b(shell.)52 b(Th)n(us,)33 b(the)g(in)n(teraction)2042
1411 < 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
1412 < Fl(i)33 b Ft(and)24 b Fl(j)36 b Ft(is)24 b(giv)n(en)f(b)n(y)h(the)2042
1413 < 2633 y(p)r(oten)n(tial)2083 2821 y Fi(u)2131 2833 y Fh(ij)2212
1414 < 2821 y Ft(=)f Fi(u)2348 2787 y Fh(LJ)2348 2841 y(ij)2439
1415 < 2821 y Ft(\()p Fi(r)2508 2833 y Fh(ij)2568 2821 y Ft(\))29
1416 < b(+)7 b Fi(u)2749 2781 y Fh(dp)2749 2844 y(ij)2822 2821
1417 < y Ft(\()p Fg(r)2893 2833 y Fh(ij)2952 2821 y Fi(;)14
1418 < b Fg(\012)3058 2833 y Fh(i)3085 2821 y Fi(;)g Fg(\012)3191
1419 < 2833 y Fh(j)3226 2821 y Ft(\))30 b(+)7 b Fi(u)3408 2781
1420 < y Fh(sp)3408 2844 y(ij)3477 2821 y Ft(\()p Fg(r)3548
1421 < 2833 y Fh(ij)3607 2821 y Fi(;)14 b Fg(\012)3713 2833
1422 < y Fh(i)3740 2821 y Fi(;)g Fg(\012)3846 2833 y Fh(j)3881
1423 < 2821 y Ft(\))p Fi(;)42 b Ft(\(1\))2042 2999 y(where)36
1424 < b(the)i Fg(r)2483 3011 y Fh(ij)2578 2999 y Ft(is)f(the)g(p)r(osition)g
1425 < (v)n(ector)f(b)r(et)n(w)n(een)h(molecules)2042 3095 y
1426 < Fl(i)44 b Ft(and)35 b Fl(j)48 b Ft(with)36 b(magnitude)f(equal)g(to)g
1427 < (the)h(distance)f Fi(r)3823 3107 y Fh(i)3851 3095 y Fi(j)5
1428 < b Ft(,)37 b(and)2042 3190 y Fg(\012)2111 3202 y Fh(i)2175
1429 < 3190 y Ft(and)g Fg(\012)2415 3202 y Fh(j)2486 3190 y
1430 < Ft(represen)n(t)f(the)h(orien)n(tations)e(of)i(the)g(resp)r(ectiv)n(e)
1431 < 2042 3286 y(molecules.)47 b(The)32 b(Lennard-Jones,)e(dip)r(ole,)i(and)
1432 < f(stic)n(ky)g(parts)2042 3381 y(of)c(the)h(p)r(oten)n(tial)g(are)e
1411 > 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
1412 > 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
1413 > 2628 y(p)r(oten)n(tial)2083 2815 y Fj(u)2131 2827 y Fi(ij)2212
1414 > 2815 y Fu(=)f Fj(u)2348 2781 y Fi(LJ)2348 2836 y(ij)2439
1415 > 2815 y Fu(\()p Fj(r)2508 2827 y Fi(ij)2568 2815 y Fu(\))29
1416 > b(+)7 b Fj(u)2749 2775 y Fi(dp)2749 2838 y(ij)2822 2815
1417 > y Fu(\()p Fh(r)2893 2827 y Fi(ij)2952 2815 y Fj(;)14
1418 > b Fh(\012)3058 2827 y Fi(i)3085 2815 y Fj(;)g Fh(\012)3191
1419 > 2827 y Fi(j)3226 2815 y Fu(\))30 b(+)7 b Fj(u)3408 2775
1420 > y Fi(sp)3408 2838 y(ij)3477 2815 y Fu(\()p Fh(r)3548
1421 > 2827 y Fi(ij)3607 2815 y Fj(;)14 b Fh(\012)3713 2827
1422 > y Fi(i)3740 2815 y Fj(;)g Fh(\012)3846 2827 y Fi(j)3881
1423 > 2815 y Fu(\))p Fj(;)42 b Fu(\(1\))2042 2994 y(where)36
1424 > b(the)i Fh(r)2483 3006 y Fi(ij)2578 2994 y Fu(is)f(the)g(p)r(osition)g
1425 > (v)n(ector)f(b)r(et)n(w)n(een)h(molecules)2042 3089 y
1426 > Fm(i)44 b Fu(and)35 b Fm(j)48 b Fu(with)36 b(magnitude)f(equal)g(to)g
1427 > (the)h(distance)f Fj(r)3823 3101 y Fi(i)3851 3089 y Fj(j)5
1428 > b Fu(,)37 b(and)2042 3185 y Fh(\012)2111 3197 y Fi(i)2175
1429 > 3185 y Fu(and)g Fh(\012)2415 3197 y Fi(j)2486 3185 y
1430 > Fu(represen)n(t)f(the)h(orien)n(tations)e(of)i(the)g(resp)r(ectiv)n(e)
1431 > 2042 3280 y(molecules.)47 b(The)32 b(Lennard-Jones,)e(dip)r(ole,)i(and)
1432 > f(stic)n(ky)g(parts)2042 3376 y(of)c(the)h(p)r(oten)n(tial)g(are)e
1433   (giving)h(b)n(y)h(the)g(follo)n(wing)e(equations,)2404
1434 < 3634 y Fi(u)2452 3600 y Fh(LJ)2452 3654 y(ij)2543 3634
1435 < y Ft(\()p Fi(r)2612 3646 y Fh(ij)2671 3634 y Ft(\))e(=)e(4)p
1436 < Fi(\017)2904 3492 y Ff(")2952 3517 y(\022)3046 3578 y
1437 < Fi(\033)p 3023 3615 96 4 v 3023 3691 a(r)3060 3703 y
1438 < Fh(ij)3129 3517 y Ff(\023)3190 3534 y Fm(12)3279 3634
1439 < y Fe(\000)3362 3517 y Ff(\022)3455 3578 y Fi(\033)p 3433
1440 < 3615 V 3433 3691 a(r)3470 3703 y Fh(ij)3539 3517 y Ff(\023)3600
1441 < 3534 y Fm(6)3637 3492 y Ff(#)3699 3634 y Fi(;)256 b Ft(\(2\))2398
1442 < 4038 y Fi(u)2446 3998 y Fh(dp)2446 4061 y(ij)2542 4038
1443 < y Ft(=)2639 3974 y Fd(\026)2698 3995 y Fh(i)2744 3974
1444 < y Fe(\001)19 b Fd(\026)2844 3995 y Fh(j)p 2639 4019 241
1445 < 4 v 2711 4095 a Fi(r)2750 4067 y Fm(3)2748 4118 y Fh(ij)2908
1446 < 4038 y Fe(\000)3001 3974 y Ft(3\()p Fd(\026)3133 3995
1447 < y Fh(i)3179 3974 y Fe(\001)g Fg(r)3260 3986 y Fh(ij)3319
1448 < 3974 y Ft(\)\()p Fd(\026)3442 3995 y Fh(j)3495 3974 y
1449 < Fe(\001)g Fg(r)3576 3986 y Fh(ij)3635 3974 y Ft(\))p
1450 < 3001 4019 667 4 v 3286 4095 a Fi(r)3325 4067 y Fm(5)3323
1451 < 4118 y Fh(ij)3705 4038 y Fi(;)250 b Ft(\(3\))2271 4396
1452 < y Fi(u)2319 4356 y Fh(sp)2319 4419 y(ij)2388 4396 y Ft(\()p
1453 < Fg(r)2459 4408 y Fh(ij)2518 4396 y Fi(;)14 b Fg(\012)2624
1454 < 4408 y Fh(i)2652 4396 y Fi(;)g Fg(\012)2757 4408 y Fh(j)2792
1455 < 4396 y Ft(\))24 b(=)2945 4340 y Fi(\027)2986 4352 y Fm(0)p
1456 < 2945 4377 79 4 v 2964 4453 a Ft(2)3034 4396 y([)p Fi(s)p
1457 < Ft(\()p Fi(r)3165 4408 y Fh(ij)3224 4396 y Ft(\))p Fi(w)r
1458 < Ft(\()p Fg(r)3388 4408 y Fh(ij)3448 4396 y Fi(;)14 b
1459 < Fg(\012)3554 4408 y Fh(i)3581 4396 y Fi(;)g Fg(\012)3687
1460 < 4408 y Fh(j)3722 4396 y Ft(\))2954 4553 y(+)k Fi(s)3076
1461 < 4519 y Fs(0)3099 4553 y Ft(\()p Fi(r)3168 4565 y Fh(ij)3227
1462 < 4553 y Ft(\))p Fi(w)3320 4519 y Fs(0)3345 4553 y Ft(\()p
1463 < Fg(r)3416 4565 y Fh(ij)3475 4553 y Fi(;)c Fg(\012)3581
1464 < 4565 y Fh(i)3608 4553 y Fi(;)g Fg(\012)3714 4565 y Fh(j)3749
1465 < 4553 y Ft(\)])28 b Fi(;)3978 4464 y Ft(\(4\))2042 4731
1466 < y(where)h Fd(\026)2343 4751 y Fh(i)2400 4731 y Ft(and)g
1467 < Fd(\026)2622 4751 y Fh(j)2687 4731 y Ft(are)f(the)i(dip)r(ole)g(unit)g
1468 < (v)n(ectors)e(of)i(particles)2042 4826 y Fl(i)35 b Ft(and)27
1469 < b Fl(j)39 b Ft(with)27 b(magnitude)g(2.35)e(D,)i Fi(\027)3253
1470 < 4838 y Fm(0)3317 4826 y Ft(scales)f(the)h(strength)f(of)2042
1471 < 4922 y(the)j(o)n(v)n(erall)d(stic)n(ky)i(p)r(oten)n(tial,)h
1472 < Fi(s)g Ft(and)f Fi(s)3335 4891 y Fs(0)3387 4922 y Ft(are)g(cubic)h
1473 < (switc)n(hing)2042 5017 y(functions.)71 b(The)39 b Fi(w)j
1474 < Ft(and)d Fi(w)2983 4987 y Fs(0)3046 5017 y Ft(functions)h(tak)n(e)e
1475 < (the)h(follo)n(wing)2042 5112 y(forms,)2362 5291 y Fi(w)r
1476 < Ft(\()p Fg(r)2494 5303 y Fh(ij)2554 5291 y Fi(;)14 b
1477 < Fg(\012)2659 5303 y Fh(i)2687 5291 y Fi(;)g Fg(\012)2793
1478 < 5303 y Fh(j)2828 5291 y Ft(\))23 b(=)g(sin)14 b Fi(\022)3126
1479 < 5303 y Fh(ij)3198 5291 y Ft(sin)g(2)p Fi(\022)3395 5303
1480 < y Fh(ij)3467 5291 y Ft(cos)f(2)p Fi(\036)3683 5303 y
1481 < Fh(ij)3741 5291 y Fi(;)214 b Ft(\(5\))2083 5561 y Fi(w)2144
1482 < 5527 y Fs(0)2168 5561 y Ft(\()p Fg(r)2239 5573 y Fh(ij)2298
1483 < 5561 y Fi(;)14 b Fg(\012)2404 5573 y Fh(i)2432 5561 y
1484 < Fi(;)g Fg(\012)2538 5573 y Fh(j)2573 5561 y Ft(\))23
1485 < b(=)g(\(cos)13 b Fi(\022)2912 5573 y Fh(ij)2978 5561
1486 < y Fe(\000)7 b Ft(0)p Fi(:)p Ft(6\))3189 5527 y Fm(2)3225
1487 < 5561 y Ft(\(cos)14 b Fi(\022)3422 5573 y Fh(ij)3488 5561
1488 < y Ft(+)7 b(0)p Fi(:)p Ft(8\))3699 5527 y Fm(2)3743 5561
1489 < y Fe(\000)g Fi(w)3876 5527 y Fm(0)3913 5561 y Fi(;)42
1490 < b Ft(\(6\))p eop
1434 > 3628 y Fj(u)2452 3594 y Fi(LJ)2452 3649 y(ij)2543 3628
1435 > y Fu(\()p Fj(r)2612 3640 y Fi(ij)2671 3628 y Fu(\))e(=)e(4)p
1436 > Fj(\017)2904 3486 y Fg(")2952 3511 y(\022)3046 3572 y
1437 > Fj(\033)p 3023 3609 96 4 v 3023 3685 a(r)3060 3697 y
1438 > Fi(ij)3129 3511 y Fg(\023)3190 3529 y Fn(12)3279 3628
1439 > y Ff(\000)3362 3511 y Fg(\022)3455 3572 y Fj(\033)p 3433
1440 > 3609 V 3433 3685 a(r)3470 3697 y Fi(ij)3539 3511 y Fg(\023)3600
1441 > 3529 y Fn(6)3637 3486 y Fg(#)3699 3628 y Fj(;)256 b Fu(\(2\))2398
1442 > 4033 y Fj(u)2446 3993 y Fi(dp)2446 4056 y(ij)2542 4033
1443 > y Fu(=)2639 3969 y Fe(\026)2698 3989 y Fi(i)2744 3969
1444 > y Ff(\001)19 b Fe(\026)2844 3989 y Fi(j)p 2639 4014 241
1445 > 4 v 2711 4090 a Fj(r)2750 4061 y Fn(3)2748 4113 y Fi(ij)2908
1446 > 4033 y Ff(\000)3001 3969 y Fu(3\()p Fe(\026)3133 3989
1447 > y Fi(i)3179 3969 y Ff(\001)g Fh(r)3260 3981 y Fi(ij)3319
1448 > 3969 y Fu(\)\()p Fe(\026)3442 3989 y Fi(j)3495 3969 y
1449 > Ff(\001)g Fh(r)3576 3981 y Fi(ij)3635 3969 y Fu(\))p
1450 > 3001 4014 667 4 v 3286 4090 a Fj(r)3325 4061 y Fn(5)3323
1451 > 4113 y Fi(ij)3705 4033 y Fj(;)250 b Fu(\(3\))2271 4390
1452 > y Fj(u)2319 4351 y Fi(sp)2319 4414 y(ij)2388 4390 y Fu(\()p
1453 > Fh(r)2459 4402 y Fi(ij)2518 4390 y Fj(;)14 b Fh(\012)2624
1454 > 4402 y Fi(i)2652 4390 y Fj(;)g Fh(\012)2757 4402 y Fi(j)2792
1455 > 4390 y Fu(\))24 b(=)2945 4334 y Fj(\027)2986 4346 y Fn(0)p
1456 > 2945 4371 79 4 v 2964 4447 a Fu(2)3034 4390 y([)p Fj(s)p
1457 > Fu(\()p Fj(r)3165 4402 y Fi(ij)3224 4390 y Fu(\))p Fj(w)r
1458 > Fu(\()p Fh(r)3388 4402 y Fi(ij)3448 4390 y Fj(;)14 b
1459 > Fh(\012)3554 4402 y Fi(i)3581 4390 y Fj(;)g Fh(\012)3687
1460 > 4402 y Fi(j)3722 4390 y Fu(\))2954 4547 y(+)k Fj(s)3076
1461 > 4513 y Ft(0)3099 4547 y Fu(\()p Fj(r)3168 4559 y Fi(ij)3227
1462 > 4547 y Fu(\))p Fj(w)3320 4513 y Ft(0)3345 4547 y Fu(\()p
1463 > Fh(r)3416 4559 y Fi(ij)3475 4547 y Fj(;)c Fh(\012)3581
1464 > 4559 y Fi(i)3608 4547 y Fj(;)g Fh(\012)3714 4559 y Fi(j)3749
1465 > 4547 y Fu(\)])28 b Fj(;)3978 4458 y Fu(\(4\))2042 4725
1466 > y(where)h Fe(\026)2343 4745 y Fi(i)2400 4725 y Fu(and)g
1467 > Fe(\026)2622 4745 y Fi(j)2687 4725 y Fu(are)f(the)i(dip)r(ole)g(unit)g
1468 > (v)n(ectors)e(of)i(particles)2042 4821 y Fm(i)35 b Fu(and)27
1469 > b Fm(j)39 b Fu(with)27 b(magnitude)g(2.35)e(D,)i Fj(\027)3253
1470 > 4833 y Fn(0)3317 4821 y Fu(scales)f(the)h(strength)f(of)2042
1471 > 4916 y(the)j(o)n(v)n(erall)d(stic)n(ky)i(p)r(oten)n(tial,)h
1472 > Fj(s)g Fu(and)f Fj(s)3335 4886 y Ft(0)3387 4916 y Fu(are)g(cubic)h
1473 > (switc)n(hing)2042 5011 y(functions.)71 b(The)39 b Fj(w)j
1474 > Fu(and)d Fj(w)2983 4981 y Ft(0)3046 5011 y Fu(functions)h(tak)n(e)e
1475 > (the)h(follo)n(wing)2042 5107 y(forms,)2362 5285 y Fj(w)r
1476 > Fu(\()p Fh(r)2494 5297 y Fi(ij)2554 5285 y Fj(;)14 b
1477 > Fh(\012)2659 5297 y Fi(i)2687 5285 y Fj(;)g Fh(\012)2793
1478 > 5297 y Fi(j)2828 5285 y Fu(\))23 b(=)g(sin)14 b Fj(\022)3126
1479 > 5297 y Fi(ij)3198 5285 y Fu(sin)g(2)p Fj(\022)3395 5297
1480 > y Fi(ij)3467 5285 y Fu(cos)f(2)p Fj(\036)3683 5297 y
1481 > Fi(ij)3741 5285 y Fj(;)214 b Fu(\(5\))2083 5555 y Fj(w)2144
1482 > 5521 y Ft(0)2168 5555 y Fu(\()p Fh(r)2239 5567 y Fi(ij)2298
1483 > 5555 y Fj(;)14 b Fh(\012)2404 5567 y Fi(i)2432 5555 y
1484 > Fj(;)g Fh(\012)2538 5567 y Fi(j)2573 5555 y Fu(\))23
1485 > b(=)g(\(cos)13 b Fj(\022)2912 5567 y Fi(ij)2978 5555
1486 > y Ff(\000)7 b Fu(0)p Fj(:)p Fu(6\))3189 5521 y Fn(2)3225
1487 > 5555 y Fu(\(cos)14 b Fj(\022)3422 5567 y Fi(ij)3488 5555
1488 > y Fu(+)7 b(0)p Fj(:)p Fu(8\))3699 5521 y Fn(2)3743 5555
1489 > y Ff(\000)g Fj(w)3876 5521 y Fn(0)3913 5555 y Fj(;)42
1490 > b Fu(\(6\))p eop
1491   %%Page: 2 2
1492 < 2 1 bop 4043 -299 a Ft(2)-150 -83 y(where)31 b Fi(w)155
1493 < -113 y Fm(0)222 -83 y Ft(=)e(0)p Fi(:)p Ft(07715.)46
1494 < b(The)31 b Fi(w)j Ft(function)e(is)g(the)g(tetrahedral)-150
1492 > 2 1 bop 4043 -299 a Fu(2)-150 -83 y(where)31 b Fj(w)155
1493 > -113 y Fn(0)222 -83 y Fu(=)e(0)p Fj(:)p Fu(07715.)46
1494 > b(The)31 b Fj(w)j Fu(function)e(is)g(the)g(tetrahedral)-150
1495   12 y(attractiv)n(e)h(term)g(that)h(promotes)f(h)n(ydrogen)f(b)r(onding)
1496   i(orien-)-150 108 y(tations)22 b(within)h(the)g(\014rst)f(solv)-5
1497 < b(ation)21 b(shell,)j(and)e Fi(w)1448 78 y Fs(0)1494
1498 < 108 y Ft(is)g(a)g(dip)r(olar)-150 203 y(repulsion)41
1497 > b(ation)21 b(shell,)j(and)e Fj(w)1448 78 y Ft(0)1494
1498 > 108 y Fu(is)g(a)g(dip)r(olar)-150 203 y(repulsion)41
1499   b(term)g(that)h(rep)r(els)f(unrealistic)g(dip)r(olar)g(arrange-)-150
1500   299 y(men)n(ts)35 b(within)g(the)h(\014rst)e(solv)-5
1501   b(ation)34 b(shell.)59 b(A)35 b(more)f(detailed)-150
1502   394 y(description)e(of)h(the)g(functional)f(parts)g(and)h(v)-5
1503   b(ariables)31 b(in)i(this)-150 490 y(p)r(oten)n(tial)28
1504   b(can)f(b)r(e)h(found)g(in)g(other)f(articles.)1296 460
1505 < y Fm(5)o(,8)-67 585 y Ft(Being)21 b(that)h(this)h(is)e(a)h(one-site)f
1505 > y Fn(5)o(,8)-67 585 y Fu(Being)21 b(that)h(this)h(is)e(a)h(one-site)f
1506   (p)r(oin)n(t)h(dip)r(ole)g(mo)r(del,)h(the)f(ac-)-150
1507   681 y(tual)28 b(force)e(calculations)h(are)f(simpli\014ed)i
1508   (signi\014can)n(tly)-7 b(.)36 b(In)28 b(the)-150 776
1509   y(original)20 b(Mon)n(te)i(Carlo)e(sim)n(ulations)h(using)g(this)h(mo)r
1510 < (del,)h(Ic)n(hiy)n(e)-150 872 y Fl(et)31 b(al.)45 b Ft(rep)r(orted)29
1510 > (del,)h(Ic)n(hiy)n(e)-150 872 y Fm(et)31 b(al.)45 b Fu(rep)r(orted)29
1511   b(a)g(calculation)g(sp)r(eed)h(up)g(of)g(up)g(to)f(an)h(order)-150
1512   967 y(of)d(magnitude)g(o)n(v)n(er)e(other)h(comparable)g(mo)r(dels)h
1513   (while)g(main-)-150 1063 y(taining)f(the)h(structural)f(b)r(eha)n(vior)
1514 < g(of)g(w)n(ater.)1312 1033 y Fm(5)1375 1063 y Ft(In)h(the)g(original)
1514 > g(of)g(w)n(ater.)1312 1033 y Fn(5)1375 1063 y Fu(In)h(the)g(original)
1515   -150 1158 y(molecular)35 b(dynamics)h(studies)h(of)g(SSD,)g(it)g(w)n
1516   (as)e(sho)n(wn)h(that)-150 1254 y(it)f(actually)e(impro)n(v)n(es)g(up)r
1517   (on)h(the)h(prediction)f(of)g(w)n(ater's)f(dy-)-150 1349
1518   y(namical)19 b(prop)r(erties)g(3)h(and)f(4-p)r(oin)n(t)h(mo)r(dels.)
1519 < 1303 1319 y Fm(8)1360 1349 y Ft(This)g(attractiv)n(e)-150
1519 > 1303 1319 y Fn(8)1360 1349 y Fu(This)g(attractiv)n(e)-150
1520   1445 y(com)n(bination)33 b(of)i(sp)r(eed)f(and)g(accurate)f(depiction)h
1521   (of)h(solv)n(en)n(t)-150 1540 y(prop)r(erties)24 b(mak)n(es)h(SSD)h(a)e
1522   (mo)r(del)i(of)f(in)n(terest)g(for)g(the)g(sim)n(ula-)-150
1523   1636 y(tion)k(of)g(large)e(scale)h(biological)f(systems,)i(suc)n(h)f
1524   (as)g(mem)n(brane)-150 1731 y(phase)f(b)r(eha)n(vior,)f(a)i(sp)r
1525   (eci\014c)f(in)n(terest)g(within)i(our)e(group.)-67 1826
1526 < y(Up)h(to)g(this)g(p)r(oin)n(t,)g(a)g(detailed)f(lo)r(ok)g(at)h(the)g
1527 < (mo)r(del's)g(struc-)-150 1922 y(ture)j(and)h(ion)f(solv)-5
1526 > y(One)33 b(of)g(the)h(k)n(ey)f(limitations)g(of)g(this)h(w)n(ater)e(mo)
1527 > r(del,)j(ho)n(w-)-150 1922 y(ev)n(er,)c(is)g(that)h(it)g(has)f(b)r(een)
1528 > g(parameterized)f(for)h(use)g(with)h(the)-150 2017 y(Ew)n(ald)22
1529 > b(Sum)h(tec)n(hnique)g(for)g(the)g(handling)g(long-ranged)d(in)n(ter-)
1530 > -150 2113 y(actions.)56 b(When)35 b(studying)f(v)n(ery)f(large)g
1531 > (systems,)j(the)e(Ew)n(ald)-150 2208 y(summation)d(and)h(ev)n(en)f
1532 > (particle-mesh)g(Ew)n(ald)g(b)r(ecome)g(com-)-150 2304
1533 > y(putational)37 b(burdens)f(with)i(their)f(resp)r(ectiv)n(e)f(ideal)g
1534 > Fj(N)1679 2251 y Fd(3)p 1679 2260 29 3 v 1679 2294 a(2)1759
1535 > 2304 y Fu(and)-150 2399 y Fj(N)23 b Fu(log)14 b Fj(N)36
1536 > b Fu(calculation)27 b(scaling)f(orders)g(for)h Fj(N)37
1537 > b Fu(particles.)1666 2369 y Fn(9)-67 2495 y Fu(Up)28
1538 > b(to)g(this)g(p)r(oin)n(t,)g(a)g(detailed)f(lo)r(ok)g(at)h(the)g(mo)r
1539 > (del's)g(struc-)-150 2590 y(ture)j(and)h(ion)f(solv)-5
1540   b(ation)31 b(abilities)g(has)g(b)r(een)h(p)r(erformed.)1748
1541 < 1892 y Fm(5)1816 1922 y Ft(In)-150 2017 y(addition,)21
1541 > 2560 y Fn(5)1816 2590 y Fu(In)-150 2686 y(addition,)21
1542   b(a)e(thorough)e(in)n(v)n(estigation)h(of)h(the)h(dynamic)f(prop)r(er-)
1543 < -150 2113 y(ties)26 b(of)g(SSD)g(w)n(as)f(p)r(erformed)h(b)n(y)f
1544 < (Chandra)g(and)h(Ic)n(hiy)n(e)f(fo)r(cus-)-150 2208 y(ing)33
1543 > -150 2781 y(ties)26 b(of)g(SSD)g(w)n(as)f(p)r(erformed)h(b)n(y)f
1544 > (Chandra)g(and)h(Ic)n(hiy)n(e)f(fo)r(cus-)-150 2877 y(ing)33
1545   b(on)g(translational)e(and)i(orien)n(tational)f(prop)r(erties)g(at)h
1546 < (298)-150 2304 y(K.)-62 2274 y Fm(8)0 2304 y Ft(This)25
1546 > (298)-150 2972 y(K.)-62 2942 y Fn(8)0 2972 y Fu(This)25
1547   b(study)g(fo)r(cuses)f(on)h(determining)f(the)h(densit)n(y)g(maxi-)-150
1548 < 2399 y(m)n(um)e(for)f(SSD)i(utilizing)f(b)r(oth)g(micro)r(canonical)f
1549 < (and)g(isobaric-)-150 2495 y(isothermal)e(ensem)n(ble)i(molecular)e
1550 < (dynamics,)i(while)g(using)f(the)-150 2590 y(reaction)37
1548 > 3068 y(m)n(um)e(for)f(SSD)i(utilizing)f(b)r(oth)g(micro)r(canonical)f
1549 > (and)g(isobaric-)-150 3163 y(isothermal)e(ensem)n(ble)i(molecular)e
1550 > (dynamics,)i(while)g(using)f(the)-150 3259 y(reaction)37
1551   b(\014eld)i(metho)r(d)g(for)f(handling)g(long-ranged)e(dip)r(olar)-150
1552 < 2686 y(in)n(teractions.)74 b(A)41 b(reaction)e(\014eld)i(metho)r(d)g
1553 < (has)e(b)r(een)i(previ-)-150 2781 y(ously)e(implemen)n(ted)g(in)h(Mon)n
1554 < (te)f(Carlo)f(sim)n(ulations)g(b)n(y)h(Liu)-150 2877
1552 > 3354 y(in)n(teractions.)74 b(A)41 b(reaction)e(\014eld)i(metho)r(d)g
1553 > (has)e(b)r(een)i(previ-)-150 3450 y(ously)e(implemen)n(ted)g(in)h(Mon)n
1554 > (te)f(Carlo)f(sim)n(ulations)g(b)n(y)h(Liu)-150 3545
1555   y(and)i(Ic)n(hiy)n(e)f(in)h(order)f(to)g(study)h(the)h(static)e
1556 < (dielectric)h(con-)-150 2972 y(stan)n(t)33 b(for)f(the)h(mo)r(del.)588
1557 < 2942 y Fm(9)659 2972 y Ft(This)f(pap)r(er)h(will)g(expand)g(the)g(scop)
1558 < r(e)-150 3068 y(of)27 b(these)g(original)f(sim)n(ulations)g(to)h(lo)r
1559 < (ok)f(on)h(ho)n(w)f(the)i(reaction)-150 3163 y(\014eld)h(a\013ects)f
1560 < (the)h(ph)n(ysical)f(and)g(dynamic)h(prop)r(erties)e(of)i(SSD)-150
1561 < 3259 y(systems.)552 3535 y Fn(I)r(I.)89 b(METHODS)-67
1562 < 3748 y Ft(As)50 b(stated)h(previously)-7 b(,)55 b(in)50
1563 < b(this)h(study)f(the)h(long-range)-150 3844 y(dip)r(ole-dip)r(ole)37
1556 > (dielectric)h(con-)-150 3641 y(stan)n(t)29 b(for)g(the)g(mo)r(del.)577
1557 > 3610 y Fn(10)677 3641 y Fu(This)g(pap)r(er)g(will)g(expand)g(the)h
1558 > (scop)r(e)-150 3736 y(of)d(these)g(original)f(sim)n(ulations)g(to)h(lo)
1559 > r(ok)f(on)h(ho)n(w)f(the)i(reaction)-150 3831 y(\014eld)h(a\013ects)f
1560 > (the)h(ph)n(ysical)f(and)g(dynamic)h(prop)r(erties)e(of)i(SSD)-150
1561 > 3927 y(systems.)552 4203 y Fo(I)r(I.)89 b(METHODS)-67
1562 > 4417 y Fu(As)50 b(stated)h(previously)-7 b(,)55 b(in)50
1563 > b(this)h(study)f(the)h(long-range)-150 4512 y(dip)r(ole-dip)r(ole)37
1564   b(in)n(teractions)f(w)n(ere)g(accoun)n(ted)h(for)f(using)h(the)-150
1565 < 3939 y(reaction)h(\014eld)h(metho)r(d.)70 b(The)39 b(magnitude)g(of)f
1566 < (the)i(reaction)-150 4035 y(\014eld)28 b(acting)f(on)g(dip)r(ole)h
1567 < Fl(i)37 b Ft(is)27 b(giv)n(en)g(b)n(y)303 4261 y Fe(E)347
1568 < 4273 y Fh(i)397 4261 y Ft(=)495 4205 y(2\()p Fi(")608
1569 < 4217 y Fh(s)661 4205 y Fe(\000)18 b Ft(1\))p 495 4242
1570 < 324 4 v 527 4318 a(2)p Fi(")608 4330 y Fh(s)661 4318
1571 < y Ft(+)g(1)856 4205 y(1)p 838 4242 78 4 v 838 4318 a
1572 < Fi(r)877 4294 y Fm(3)875 4338 y Fh(c)945 4182 y Ff(X)939
1573 < 4360 y Fh(j)s Fs(2R)1085 4261 y Fd(\026)1144 4281 y Fh(j)1179
1574 < 4261 y Fi(f)9 b Ft(\()p Fi(r)1298 4273 y Fh(ij)1357 4261
1575 < y Ft(\))28 b Fi(;)346 b Ft(\(7\))-150 4533 y(where)32
1576 < b Fe(R)h Ft(is)f(the)h(ca)n(vit)n(y)e(de\014ned)h(b)n(y)h(the)f
1577 < (cuto\013)h(radius)e(\()p Fi(r)1802 4545 y Fh(c)1837
1578 < 4533 y Ft(\),)-150 4629 y Fi(")-111 4641 y Fh(s)-43 4629
1579 < y Ft(is)i(the)h(dielectric)f(constan)n(t)f(imp)r(osed)h(on)g(the)g
1580 < (system)g(\(80)-150 4724 y(in)k(this)f(case\),)i Fd(\026)427
1581 < 4744 y Fh(j)499 4724 y Ft(is)e(the)h(dip)r(ole)f(momen)n(t)h(v)n(ector)
1582 < e(of)h(parti-)-150 4832 y(cle)43 b Fl(j)p Ft(,)48 b(and)43
1583 < b Fi(f)9 b Ft(\()p Fi(r)382 4844 y Fh(ij)441 4832 y Ft(\))43
1584 < b(is)g(a)g(cubic)g(switc)n(hing)g(function.)1635 4801
1585 < y Fm(10)1749 4832 y Ft(The)-150 4927 y(reaction)c(\014eld)h(con)n
1586 < (tribution)g(to)g(the)g(total)g(energy)f(b)n(y)h(par-)-150
1587 < 5022 y(ticle)f Fl(i)47 b Ft(is)38 b(giv)n(en)g(b)n(y)g
1588 < Fe(\000)636 4990 y Fm(1)p 636 5004 34 4 v 636 5051 a(2)679
1589 < 5022 y Fd(\026)737 5043 y Fh(i)791 5022 y Fe(\001)25
1590 < b(E)883 5034 y Fh(i)949 5022 y Ft(and)39 b(the)f(torque)g(on)g(dip)r
1591 < (ole)-150 5127 y Fl(i)47 b Ft(b)n(y)38 b Fd(\026)107
1592 < 5147 y Fh(i)160 5127 y Fe(\002)25 b(E)294 5139 y Fh(i)321
1593 < 5127 y Ft(.)344 5097 y Fm(10)453 5127 y Ft(Use)38 b(of)g(reaction)f
1594 < (\014eld)h(is)g(kno)n(wn)f(to)h(alter)-150 5222 y(the)28
1595 < b(orien)n(tational)e(dynamic)i(prop)r(erties,)f(suc)n(h)g(as)h(the)g
1596 < (dielec-)-150 5318 y(tric)35 b(relaxation)f(time,)39
1597 < b(based)c(on)g(c)n(hanges)f(in)i(the)g(length)f(of)2042
1598 < -83 y(the)h(cuto\013)g(radius.)2680 -113 y Fm(11)2786
1599 < -83 y Ft(This)f(v)-5 b(ariable)35 b(b)r(eha)n(vior)g(mak)n(es)g(reac-)
1600 < 2042 12 y(tion)e(\014eld)h(a)f(less)h(attractiv)n(e)e(metho)r(d)i(than)
1601 < g(other)f(metho)r(ds,)2042 108 y(lik)n(e)h(the)h(Ew)n(ald)e(summation;)
1602 < 38 b(ho)n(w)n(ev)n(er,)d(for)f(the)h(sim)n(ulation)2042
1603 < 203 y(of)e(large-scale)e(system,)k(the)f(computational)f(cost)g(b)r
1586 < (ene\014t)h(of)2042 299 y(reaction)19 b(\014eld)h(is)h(dramatic.)33
1565 > 4608 y(reaction)h(\014eld)h(metho)r(d.)70 b(The)39 b(magnitude)g(of)f
1566 > (the)i(reaction)-150 4703 y(\014eld)28 b(acting)f(on)g(dip)r(ole)h
1567 > Fm(i)37 b Fu(is)27 b(giv)n(en)g(b)n(y)303 4929 y Ff(E)347
1568 > 4941 y Fi(i)397 4929 y Fu(=)495 4873 y(2\()p Fj(")608
1569 > 4885 y Fi(s)661 4873 y Ff(\000)18 b Fu(1\))p 495 4910
1570 > 324 4 v 527 4986 a(2)p Fj(")608 4998 y Fi(s)661 4986
1571 > y Fu(+)g(1)856 4873 y(1)p 838 4910 78 4 v 838 4986 a
1572 > Fj(r)877 4962 y Fn(3)875 5006 y Fi(c)945 4850 y Fg(X)939
1573 > 5028 y Fi(j)s Ft(2R)1085 4929 y Fe(\026)1144 4949 y Fi(j)1179
1574 > 4929 y Fj(f)9 b Fu(\()p Fj(r)1298 4941 y Fi(ij)1357 4929
1575 > y Fu(\))28 b Fj(;)346 b Fu(\(7\))-150 5201 y(where)32
1576 > b Ff(R)h Fu(is)f(the)h(ca)n(vit)n(y)e(de\014ned)h(b)n(y)h(the)f
1577 > (cuto\013)h(radius)e(\()p Fj(r)1802 5213 y Fi(c)1837
1578 > 5201 y Fu(\),)-150 5297 y Fj(")-111 5309 y Fi(s)-43 5297
1579 > y Fu(is)i(the)h(dielectric)f(constan)n(t)f(imp)r(osed)h(on)g(the)g
1580 > (system)g(\(80)2042 -83 y(in)j(this)h(case\),)h Fe(\026)2619
1581 > -63 y Fi(j)2690 -83 y Fu(is)f(the)g(dip)r(ole)f(momen)n(t)g(v)n(ector)g
1582 > (of)g(parti-)2042 24 y(cle)43 b Fm(j)p Fu(,)48 b(and)43
1583 > b Fj(f)9 b Fu(\()p Fj(r)2574 36 y Fi(ij)2632 24 y Fu(\))44
1584 > b(is)f(a)g(cubic)g(switc)n(hing)g(function.)3827 -6 y
1585 > Fn(11)3941 24 y Fu(The)2042 120 y(reaction)c(\014eld)h(con)n(tribution)
1586 > f(to)h(the)h(total)f(energy)f(b)n(y)g(par-)2042 215 y(ticle)f
1587 > Fm(i)48 b Fu(is)38 b(giv)n(en)g(b)n(y)g Ff(\000)2828
1588 > 183 y Fn(1)p 2827 197 34 4 v 2827 244 a(2)2870 215 y
1589 > Fe(\026)2929 236 y Fi(i)2983 215 y Ff(\001)25 b(E)3075
1590 > 227 y Fi(i)3141 215 y Fu(and)38 b(the)h(torque)f(on)g(dip)r(ole)2042
1591 > 320 y Fm(i)47 b Fu(b)n(y)38 b Fe(\026)2298 340 y Fi(i)2351
1592 > 320 y Ff(\002)25 b(E)2485 332 y Fi(i)2513 320 y Fu(.)2536
1593 > 290 y Fn(11)2644 320 y Fu(Use)38 b(of)g(reaction)f(\014eld)i(is)f(kno)n
1594 > (wn)f(to)h(alter)2042 415 y(the)28 b(orien)n(tational)e(dynamic)i(prop)
1595 > r(erties,)f(suc)n(h)g(as)g(the)i(dielec-)2042 511 y(tric)35
1596 > b(relaxation)f(time,)k(based)d(on)h(c)n(hanges)e(in)i(the)g(length)f
1597 > (of)2042 606 y(the)h(cuto\013)g(radius.)2680 576 y Fn(12)2786
1598 > 606 y Fu(This)f(v)-5 b(ariable)35 b(b)r(eha)n(vior)g(mak)n(es)g(reac-)
1599 > 2042 702 y(tion)e(\014eld)h(a)f(less)h(attractiv)n(e)e(metho)r(d)i
1600 > (than)g(other)f(metho)r(ds,)2042 797 y(lik)n(e)h(the)h(Ew)n(ald)e
1601 > (summation;)38 b(ho)n(w)n(ev)n(er,)d(for)f(the)h(sim)n(ulation)2042
1602 > 893 y(of)e(large-scale)e(system,)k(the)f(computational)f(cost)g(b)r
1603 > (ene\014t)h(of)2042 988 y(reaction)19 b(\014eld)h(is)h(dramatic.)33
1604   b(T)-7 b(o)20 b(address)f(some)h(of)g(the)h(dynam-)2042
1605 < 394 y(ical)28 b(prop)r(ert)n(y)f(alterations)g(due)h(to)h(the)f(use)g
1606 < (of)h(reaction)e(\014eld,)2042 490 y(sim)n(ulations)33
1605 > 1084 y(ical)28 b(prop)r(ert)n(y)f(alterations)g(due)h(to)h(the)f(use)g
1606 > (of)h(reaction)e(\014eld,)2042 1179 y(sim)n(ulations)33
1607   b(w)n(ere)g(also)g(p)r(erformed)g(without)h(a)g(surrounding)2042
1608 < 585 y(dielectric)c(and)f(suggestions)g(are)g(prop)r(osed)g(on)h(ho)n(w)
1609 < f(to)h(mak)n(e)2042 681 y(SSD)e(more)f(compatible)g(with)h(a)g
1610 < (reaction)e(\014eld.)2125 776 y(Sim)n(ulations)57 b(w)n(ere)f(p)r
1611 < (erformed)h(in)h(b)r(oth)g(the)g(isobaric-)2042 872 y(isothermal)28
1612 < b(and)g(micro)r(canonical)f(ensem)n(bles.)40 b(The)29
1613 < b(constan)n(t)2042 967 y(pressure)c(sim)n(ulations)g(w)n(ere)g
1614 < (implemen)n(ted)i(using)f(an)f(in)n(tegral)2042 1063
1608 > 1275 y(dielectric)c(and)f(suggestions)g(are)g(prop)r(osed)g(on)h(ho)n
1609 > (w)f(to)h(mak)n(e)2042 1370 y(SSD)e(more)f(compatible)g(with)h(a)g
1610 > (reaction)e(\014eld.)2125 1466 y(Sim)n(ulations)57 b(w)n(ere)f(p)r
1611 > (erformed)h(in)h(b)r(oth)g(the)g(isobaric-)2042 1561
1612 > y(isothermal)28 b(and)g(micro)r(canonical)f(ensem)n(bles.)40
1613 > b(The)29 b(constan)n(t)2042 1657 y(pressure)c(sim)n(ulations)g(w)n(ere)
1614 > g(implemen)n(ted)i(using)f(an)f(in)n(tegral)2042 1752
1615   y(thermostat)i(and)h(barostat)f(as)h(outlined)g(b)n(y)g(Ho)r(o)n(v)n
1616 < (er.)3781 1033 y Fm(12)n(,13)3963 1063 y Ft(F)-7 b(or)2042
1617 < 1158 y(the)34 b(constan)n(t)e(pressure)g(sim)n(ulations,)i(the)g
1618 < Fl(Q)41 b Ft(parameter)32 b(for)2042 1254 y(the)e(w)n(as)f(set)h(to)g
1619 < (5.0)f(am)n(u)g Fe(\001)2928 1239 y Ft(\027)2928 1254
1620 < y(A)2990 1224 y Fm(2)3028 1254 y Ft(,)h(and)g(the)g(relaxation)e(time)j
1621 < (\()p Fi(\034)9 b Ft(\))2042 1349 y(w)n(as)26 b(set)i(at)f(100)g(ps.)
1622 < 2125 1445 y(In)n(tegration)e(of)h(the)g(equations)f(of)h(motion)g(w)n
1623 < (as)f(carried)g(out)2042 1540 y(using)h(the)g(symplectic)h(splitting)g
1624 < (metho)r(d)f(prop)r(osed)g(b)n(y)g(Dull-)2042 1636 y(w)n(eb)r(er)37
1625 < b Fl(et)i(al.)p Ft(.)2508 1605 y Fm(14)2618 1636 y Ft(The)f(reason)f
1626 < (for)g(this)i(in)n(tegrator)d(selection)2042 1731 y(deals)g(with)h(p)r
1616 > (er.)3781 1722 y Fn(13)n(,14)3963 1752 y Fu(F)-7 b(or)2042
1617 > 1848 y(the)34 b(constan)n(t)e(pressure)g(sim)n(ulations,)i(the)g
1618 > Fm(Q)41 b Fu(parameter)32 b(for)2042 1943 y(the)e(w)n(as)f(set)h(to)g
1619 > (5.0)f(am)n(u)g Ff(\001)2928 1928 y Fu(\027)2928 1943
1620 > y(A)2990 1913 y Fn(2)3028 1943 y Fu(,)h(and)g(the)g(relaxation)e(time)j
1621 > (\()p Fj(\034)9 b Fu(\))2042 2038 y(w)n(as)26 b(set)i(at)f(100)g(ps.)
1622 > 2125 2134 y(In)n(tegration)e(of)h(the)g(equations)f(of)h(motion)g(w)n
1623 > (as)f(carried)g(out)2042 2229 y(using)h(the)g(symplectic)h(splitting)g
1624 > (metho)r(d)f(prop)r(osed)g(b)n(y)g(Dull-)2042 2325 y(w)n(eb)r(er)37
1625 > b Fm(et)i(al.)p Fu(.)2508 2295 y Fn(15)2618 2325 y Fu(The)f(reason)f
1626 > (for)g(this)i(in)n(tegrator)d(selection)2042 2420 y(deals)g(with)h(p)r
1627   (o)r(or)f(energy)f(conserv)-5 b(ation)36 b(of)g(rigid)g(b)r(o)r(dy)h
1628 < (sys-)2042 1826 y(tems)24 b(using)h(quaternions.)34 b(While)25
1629 < b(quaternions)e(w)n(ork)h(w)n(ell)g(for)2042 1922 y(orien)n(tational)33
1628 > (sys-)2042 2516 y(tems)24 b(using)h(quaternions.)34 b(While)25
1629 > b(quaternions)e(w)n(ork)h(w)n(ell)g(for)2042 2611 y(orien)n(tational)33
1630   b(motion)h(in)h(alternate)e(ensem)n(bles,)j(the)f(micro-)2042
1631 < 2017 y(canonical)j(ensem)n(ble)i(has)f(a)g(constan)n(t)g(energy)g
1632 < (requiremen)n(t)2042 2113 y(that)27 b(is)h(actually)f(quite)g(sensitiv)
1633 < n(e)g(to)g(errors)f(in)h(the)h(equations)2042 2208 y(of)e(motion.)37
1631 > 2707 y(canonical)j(ensem)n(ble)i(has)f(a)g(constan)n(t)g(energy)g
1632 > (requiremen)n(t)2042 2802 y(that)27 b(is)h(actually)f(quite)g(sensitiv)
1633 > n(e)g(to)g(errors)f(in)h(the)h(equations)2042 2898 y(of)e(motion.)37
1634   b(The)27 b(original)e(implemen)n(tation)i(of)f(this)h(co)r(de)g(uti-)
1635 < 2042 2304 y(lized)19 b(quaternions)e(for)h(rotational)f(motion)i
1636 < (propagation;)g(ho)n(w-)2042 2399 y(ev)n(er,)32 b(a)g(detailed)g(in)n
1635 > 2042 2993 y(lized)19 b(quaternions)e(for)h(rotational)f(motion)i
1636 > (propagation;)g(ho)n(w-)2042 3089 y(ev)n(er,)32 b(a)g(detailed)g(in)n
1637   (v)n(estigation)f(sho)n(w)n(ed)g(that)i(they)f(resulted)2042
1638 < 2495 y(in)d(a)f(steady)g(drift)h(in)g(the)g(total)g(energy)-7
1639 < b(,)28 b(something)g(that)h(has)2042 2590 y(b)r(een)f(observ)n(ed)e(b)n
1640 < (y)h(others.)2941 2560 y Fm(15)2125 2686 y Ft(The)d(k)n(ey)g
1638 > 3184 y(in)d(a)f(steady)g(drift)h(in)g(the)g(total)g(energy)-7
1639 > b(,)28 b(something)g(that)h(has)2042 3280 y(b)r(een)f(observ)n(ed)e(b)n
1640 > (y)h(others.)2941 3250 y Fn(16)2125 3375 y Fu(The)d(k)n(ey)g
1641   (di\013erence)g(in)h(the)f(in)n(tegration)f(metho)r(d)i(prop)r(osed)
1642 < 2042 2781 y(b)n(y)37 b(Dullw)n(eb)r(er)h Fl(et)h(al.)68
1643 < b Ft(is)37 b(that)h(the)g(en)n(tire)f(rotation)g(matrix)2042
1644 < 2877 y(is)h(propagated)f(from)h(one)g(time)g(step)h(to)f(the)h(next.)69
1645 < b(In)39 b(the)2042 2972 y(past,)32 b(this)g(w)n(ould)f(not)g(ha)n(v)n
1642 > 2042 3471 y(b)n(y)37 b(Dullw)n(eb)r(er)h Fm(et)h(al.)68
1643 > b Fu(is)37 b(that)h(the)g(en)n(tire)f(rotation)g(matrix)2042
1644 > 3566 y(is)h(propagated)f(from)h(one)g(time)g(step)h(to)f(the)h(next.)69
1645 > b(In)39 b(the)2042 3662 y(past,)32 b(this)g(w)n(ould)f(not)g(ha)n(v)n
1646   (e)g(b)r(een)h(as)f(feasible)g(a)g(option,)h(b)r(e-)2042
1647 < 3068 y(ing)39 b(that)h(the)g(rotation)e(matrix)h(for)g(a)h(single)f(b)r
1648 < (o)r(dy)g(is)h(nine)2042 3163 y(elemen)n(ts)23 b(long)g(as)f(opp)r
1647 > 3757 y(ing)39 b(that)h(the)g(rotation)e(matrix)h(for)g(a)h(single)f(b)r
1648 > (o)r(dy)g(is)h(nine)2042 3853 y(elemen)n(ts)23 b(long)g(as)f(opp)r
1649   (osed)h(to)h(3)f(or)f(4)h(elemen)n(ts)g(for)g(Euler)g(an-)2042
1650 < 3259 y(gles)34 b(and)h(quaternions)f(resp)r(ectiv)n(ely)-7
1651 < b(.)59 b(System)35 b(memory)g(has)2042 3354 y(b)r(ecome)g(m)n(uc)n(h)g
1650 > 3948 y(gles)34 b(and)h(quaternions)f(resp)r(ectiv)n(ely)-7
1651 > b(.)59 b(System)35 b(memory)g(has)2042 4043 y(b)r(ecome)g(m)n(uc)n(h)g
1652   (less)f(of)h(an)g(issue)g(in)g(recen)n(t)g(times,)i(and)e(this)2042
1653 < 3450 y(has)g(resulted)g(in)h(substan)n(tial)f(b)r(ene\014ts)h(in)g
1654 < (energy)e(conserv)-5 b(a-)2042 3545 y(tion.)36 b(There)26
1653 > 4139 y(has)g(resulted)g(in)h(substan)n(tial)f(b)r(ene\014ts)h(in)g
1654 > (energy)e(conserv)-5 b(a-)2042 4234 y(tion.)36 b(There)26
1655   b(is)g(still)h(the)g(issue)e(of)i(an)f(additional)f(5)h(or)g(6)g(addi-)
1656 < 2042 3641 y(tional)21 b(elemen)n(ts)h(for)f(describing)g(the)h(orien)n
1657 < (tation)f(of)g(eac)n(h)g(par-)2042 3736 y(ticle,)i(whic)n(h)e(will)h
1656 > 2042 4330 y(tional)21 b(elemen)n(ts)h(for)f(describing)g(the)h(orien)n
1657 > (tation)f(of)g(eac)n(h)g(par-)2042 4425 y(ticle,)i(whic)n(h)e(will)h
1658   (increase)e(dump)i(\014les)g(substan)n(tially)-7 b(.)34
1659 < b(Simply)2042 3831 y(translating)24 b(the)i(rotation)f(matrix)g(in)n
1660 < (to)h(its)g(comp)r(onen)n(t)f(Euler)2042 3927 y(angles)34
1659 > b(Simply)2042 4521 y(translating)24 b(the)i(rotation)f(matrix)g(in)n
1660 > (to)h(its)g(comp)r(onen)n(t)f(Euler)2042 4616 y(angles)34
1661   b(or)h(quaternions)g(for)g(storage)f(purp)r(oses)h(reliev)n(es)f(this)
1662 < 2042 4022 y(burden.)2125 4118 y(The)22 b(symplectic)h(splitting)g
1662 > 2042 4712 y(burden.)2125 4807 y(The)22 b(symplectic)h(splitting)g
1663   (metho)r(d)g(allo)n(ws)e(for)h(V)-7 b(erlet)23 b(st)n(yle)2042
1664 < 4213 y(in)n(tegration)38 b(of)h(b)r(oth)h(linear)f(and)g(angular)f
1665 < (motion)h(of)h(rigid)2042 4309 y(b)r(o)r(dies.)93 b(In)47
1664 > 4903 y(in)n(tegration)38 b(of)h(b)r(oth)h(linear)f(and)g(angular)f
1665 > (motion)h(of)h(rigid)2042 4998 y(b)r(o)r(dies.)93 b(In)47
1666   b(the)g(in)n(tegration)e(metho)r(d,)51 b(the)c(orien)n(tational)2042
1667 < 4404 y(propagation)23 b(in)n(v)n(olv)n(es)h(a)h(sequence)g(of)h(matrix)
1668 < f(ev)-5 b(aluations)24 b(to)2042 4500 y(up)r(date)c(the)h(rotation)e
1669 < (matrix.)3026 4470 y Fm(14)3116 4500 y Ft(These)h(matrix)f(rotations)g
1670 < (end)2042 4595 y(up)33 b(b)r(eing)g(more)f(costly)g(computationally)g
1671 < (than)h(the)h(simpler)2042 4691 y(arithmetic)e(quaternion)e
1672 < (propagation.)48 b(On)32 b(a)n(v)n(erage,)e(a)h(1000)2042
1673 < 4786 y(SSD)i(particle)e(sim)n(ulation)h(sho)n(ws)f(a)h(7\045)g
1657 < (increase)f(in)h(sim)n(ula-)2042 4882 y(tion)i(time)h(using)f(the)g
1658 < (symplectic)h(step)f(metho)r(d)h(in)f(place)g(of)2042
1659 < 4977 y(quaternions.)j(This)28 b(cost)g(is)g(more)f(than)i(justi\014ed)g
1660 < (when)f(com-)2042 5073 y(paring)38 b(the)i(energy)e(conserv)-5
1661 < b(ation)38 b(of)h(the)h(t)n(w)n(o)e(metho)r(ds)i(as)2042
1662 < 5168 y(illustrated)27 b(in)h(\014gure)f(1.)2125 5264
1663 < y(In)33 b(\014gure)f(1,)h(the)h(resulting)e(energy)f(drift)j(at)e(v)-5
1664 < b(arious)32 b(time)2042 5359 y(steps)g(for)g(b)r(oth)i(the)f
1665 < (symplectic)f(step)h(and)g(quaternion)e(in)n(te-)p eop
1667 > 5094 y(propagation)23 b(in)n(v)n(olv)n(es)h(a)h(sequence)g(of)h(matrix)
1668 > f(ev)-5 b(aluations)24 b(to)2042 5189 y(up)r(date)c(the)h(rotation)e
1669 > (matrix.)3026 5159 y Fn(15)3116 5189 y Fu(These)h(matrix)f(rotations)g
1670 > (end)2042 5285 y(up)33 b(b)r(eing)g(more)f(costly)g(computationally)g
1671 > (than)h(the)h(simpler)2042 5380 y(arithmetic)e(quaternion)e
1672 > (propagation.)48 b(On)32 b(a)n(v)n(erage,)e(a)h(1000)p
1673 > eop
1674   %%Page: 3 3
1675 < 3 2 bop 4043 -299 a Ft(3)-139 -166 y
1675 > 3 2 bop 4043 -299 a Fu(3)-139 -166 y
1676   gsave currentpoint currentpoint translate -90 neg rotate neg exch
1677   neg exch translate
1678   -139 -166 a @beginspecial
# Line 12406 | Line 12414 | cleartomark countdictstack exch sub { end } repeat res
12414   %%EndDocument
12415   @endspecial 1302 -166 a
12416   currentpoint grestore moveto
12417 < 1302 -166 a -150 1418 a Fq(FIG.)26
12417 > 1302 -166 a -150 1418 a Fr(FIG.)26
12418   b(1:)34 b(Energy)26 b(conserv)l(ation)g(using)f(quaternion)h(based)f
12419   (in)n(tegra-)-150 1505 y(tion)i(v)n(ersus)g(the)f(symplectic)h(step)f
12420   (metho)r(d)g(prop)r(osed)h(b)n(y)f(Dullw)n(e-)-150 1592
12421 < y(b)r(er)h Fr(et)j(al.)39 b Fq(with)27 b(increasing)i(time)e(step.)39
12421 > y(b)r(er)h Fs(et)j(al.)39 b Fr(with)27 b(increasing)i(time)e(step.)39
12422   b(F)-6 b(or)27 b(eac)n(h)h(time)f(step,)h(the)-150 1680
12423   y(dotted)f(line)h(is)g(total)g(energy)f(using)h(the)f(symplectic)g
12424   (step)g(in)n(tegra-)-150 1767 y(tor,)h(and)e(the)h(solid)h(line)f
12425   (comes)g(from)g(the)f(quaternion)h(in)n(tegrator.)-150
12426   1854 y(The)22 b(larger)h(time)e(step)g(plots)h(are)h(shifted)f(up)e
12427   (from)i(the)f(true)g(energy)-150 1941 y(baseline)27 b(for)f(clarit)n(y)
12428 < -6 b(.)-150 2221 y Ft(gration)25 b(sc)n(hemes)h(is)g(compared.)36
12429 < b(All)27 b(of)f(the)h(1000)e(SSD)i(parti-)-150 2317 y(cle)g(sim)n
12430 < (ulations)g(started)g(with)h(the)g(same)f(con\014guration,)f(and)-150
12431 < 2412 y(the)40 b(only)f(di\013erence)h(w)n(as)f(the)h(metho)r(d)g(for)f
12432 < (handling)h(rota-)-150 2508 y(tional)i(motion.)79 b(A)n(t)42
12428 > -6 b(.)-150 2221 y Fu(SSD)33 b(particle)f(sim)n(ulation)f(sho)n(ws)g(a)
12429 > h(7\045)g(increase)f(in)h(sim)n(ula-)-150 2317 y(tion)i(time)h(using)f
12430 > (the)h(symplectic)f(step)g(metho)r(d)h(in)g(place)e(of)-150
12431 > 2412 y(quaternions.)k(This)28 b(cost)g(is)g(more)g(than)g(justi\014ed)h
12432 > (when)f(com-)-150 2508 y(paring)38 b(the)i(energy)e(conserv)-5
12433 > b(ation)38 b(of)h(the)h(t)n(w)n(o)e(metho)r(ds)i(as)-150
12434 > 2603 y(illustrated)27 b(in)h(\014gure)f(1.)-67 2699 y(In)33
12435 > b(\014gure)f(1,)i(the)f(resulting)f(energy)g(drift)h(at)f(v)-5
12436 > b(arious)32 b(time)-150 2794 y(steps)h(for)f(b)r(oth)h(the)g
12437 > (symplectic)g(step)f(and)h(quaternion)f(in)n(te-)-150
12438 > 2890 y(gration)25 b(sc)n(hemes)h(is)g(compared.)36 b(All)27
12439 > b(of)f(the)h(1000)e(SSD)i(parti-)-150 2985 y(cle)g(sim)n(ulations)g
12440 > (started)g(with)h(the)g(same)f(con\014guration,)f(and)-150
12441 > 3081 y(the)40 b(only)f(di\013erence)h(w)n(as)f(the)h(metho)r(d)g(for)f
12442 > (handling)h(rota-)-150 3176 y(tional)i(motion.)79 b(A)n(t)42
12443   b(time)h(steps)f(of)f(0.1)g(and)h(0.5)f(fs,)46 b(b)r(oth)-150
12444 < 2603 y(metho)r(ds)37 b(for)g(propagating)e(particle)h(rotation)g
12445 < (conserv)n(e)g(en-)-150 2699 y(ergy)31 b(fairly)i(w)n(ell,)g(with)g
12446 < (the)g(quaternion)f(metho)r(d)h(sho)n(wing)f(a)-150 2794
12444 > 3272 y(metho)r(ds)37 b(for)g(propagating)e(particle)h(rotation)g
12445 > (conserv)n(e)g(en-)-150 3367 y(ergy)31 b(fairly)i(w)n(ell,)g(with)g
12446 > (the)g(quaternion)f(metho)r(d)h(sho)n(wing)f(a)-150 3463
12447   y(sligh)n(t)d(energy)g(drift)h(o)n(v)n(er)d(time)j(in)g(the)g(0.5)f(fs)
12448 < h(time)g(step)g(sim-)-150 2890 y(ulation.)47 b(A)n(t)31
12448 > h(time)g(step)g(sim-)-150 3558 y(ulation.)47 b(A)n(t)31
12449   b(time)h(steps)f(of)g(1)f(and)h(2)g(fs,)h(the)f(energy)f(conser-)-150
12450 < 2985 y(v)-5 b(ation)25 b(b)r(ene\014ts)h(of)g(the)g(symplectic)f(step)h
12451 < (metho)r(d)g(are)f(clearly)-150 3081 y(demonstrated.)-67
12452 < 3176 y(Energy)e(drift)j(in)f(these)g(SSD)g(particle)g(sim)n(ulations)f
12453 < (w)n(as)f(un-)-150 3272 y(noticeable)36 b(for)h(time)g(steps)g(up)g(to)
12454 < g(three)g(fem)n(toseconds.)64 b(A)-150 3367 y(sligh)n(t)40
12450 > 3653 y(v)-5 b(ation)25 b(b)r(ene\014ts)h(of)g(the)g(symplectic)f(step)h
12451 > (metho)r(d)g(are)f(clearly)-150 3749 y(demonstrated.)-67
12452 > 3844 y(Energy)e(drift)j(in)f(these)g(SSD)g(particle)g(sim)n(ulations)f
12453 > (w)n(as)f(un-)-150 3940 y(noticeable)36 b(for)h(time)g(steps)g(up)g(to)
12454 > g(three)g(fem)n(toseconds.)64 b(A)-150 4035 y(sligh)n(t)40
12455   b(energy)f(drift)i(on)f(the)h(order)e(of)h(0.012)f(k)n(cal/mol)f(p)r
12456 < (er)-150 3463 y(nanosecond)21 b(w)n(as)h(observ)n(ed)g(at)g(a)h(time)g
12457 < (step)g(of)g(four)f(fem)n(tosec-)-150 3558 y(onds,)34
12456 > (er)-150 4131 y(nanosecond)21 b(w)n(as)h(observ)n(ed)g(at)g(a)h(time)g
12457 > (step)g(of)g(four)f(fem)n(tosec-)-150 4226 y(onds,)34
12458   b(and)f(as)g(exp)r(ected,)i(this)e(drift)h(increases)e(dramatically)
12459 < -150 3653 y(with)24 b(increasing)e(time)i(step.)35 b(T)-7
12460 < b(o)23 b(insure)g(accuracy)f(in)h(the)h(con-)-150 3749
12459 > -150 4322 y(with)24 b(increasing)e(time)i(step.)35 b(T)-7
12460 > b(o)23 b(insure)g(accuracy)f(in)h(the)h(con-)-150 4417
12461   y(stan)n(t)j(energy)f(sim)n(ulations,)h(time)h(steps)f(w)n(ere)f(set)i
12462 < (at)f(2)g(fs)h(and)-150 3844 y(k)n(ept)38 b(at)g(this)g(v)-5
12462 > (at)f(2)g(fs)h(and)-150 4513 y(k)n(ept)38 b(at)g(this)g(v)-5
12463   b(alue)38 b(for)f(constan)n(t)g(pressure)g(sim)n(ulations)g(as)-150
12464 < 3940 y(w)n(ell.)-67 4035 y(Ice)g(crystals)e(in)i(b)r(oth)g(the)h
12465 < Fi(I)886 4047 y Fh(h)966 4035 y Ft(and)f Fi(I)1173 4047
12466 < y Fh(c)1244 4035 y Ft(lattices)f(w)n(ere)g(gen-)-150
12467 < 4131 y(erated)k(as)g(starting)g(p)r(oin)n(ts)g(for)g(all)g(the)h(sim)n
12468 < (ulations.)75 b(The)-150 4226 y Fi(I)-114 4238 y Fh(h)-38
12469 < 4226 y Ft(crystals)31 b(w)n(ere)h(formed)g(b)n(y)g(\014rst)g(arranging)
12470 < e(the)j(cen)n(ter)e(of)-150 4322 y(masses)21 b(of)i(the)g(SSD)g
12464 > 4608 y(w)n(ell.)-67 4704 y(Ice)g(crystals)e(in)i(b)r(oth)g(the)h
12465 > Fj(I)886 4716 y Fi(h)966 4704 y Fu(and)f Fj(I)1173 4716
12466 > y Fi(c)1244 4704 y Fu(lattices)f(w)n(ere)g(gen-)-150
12467 > 4799 y(erated)k(as)g(starting)g(p)r(oin)n(ts)g(for)g(all)g(the)h(sim)n
12468 > (ulations.)75 b(The)-150 4895 y Fj(I)-114 4907 y Fi(h)-38
12469 > 4895 y Fu(crystals)31 b(w)n(ere)h(formed)g(b)n(y)g(\014rst)g(arranging)
12470 > e(the)j(cen)n(ter)e(of)-150 4990 y(masses)21 b(of)i(the)g(SSD)g
12471   (particles)f(in)n(to)g(a)g(\\hexagonal")e(ice)i(lattice)-150
12472 < 4417 y(of)31 b(1024)d(particles.)45 b(Because)30 b(of)h(the)g(crystal)e
12473 < (structure)h(of)h Fi(I)1849 4429 y Fh(h)-150 4513 y Ft(ice,)23
12472 > 5086 y(of)31 b(1024)d(particles.)45 b(Because)30 b(of)h(the)g(crystal)e
12473 > (structure)h(of)h Fj(I)1849 5098 y Fi(h)-150 5181 y Fu(ice,)23
12474   b(the)f(sim)n(ulation)f(b)r(o)n(x)g(assumed)g(a)g(rectangular)f(shap)r
12475 < (e)h(with)-150 4608 y(a)43 b(edge)g(length)h(ratio)e(of)i(appro)n
12476 < (ximately)d(1.00)p Fe(\002)p Ft(1.06)p Fe(\002)p Ft(1.23.)-150
12477 < 4704 y(The)e(particles)e(w)n(ere)h(then)h(allo)n(w)n(ed)e(to)i(orien)n
12478 < (t)e(freely)h(ab)r(out)-150 4799 y(\014xed)23 b(p)r(ositions)g(with)g
12461 < (angular)e(momen)n(ta)i(randomized)f(at)h(400)-150 4895
12462 < y(K)40 b(for)g(v)-5 b(arying)39 b(times.)75 b(The)41
12463 < b(rotational)d(temp)r(erature)i(w)n(as)-150 4990 y(then)g(scaled)e(do)n
12464 < (wn)h(in)g(stages)f(to)h(slo)n(wly)g(co)r(ol)f(the)i(crystals)-150
12465 < 5086 y(do)n(wn)27 b(to)g(25)f(K.)h(The)h(particles)e(w)n(ere)h(then)g
12466 < (allo)n(w)n(ed)f(translate)-150 5181 y(with)35 b(\014xed)f(orien)n
12467 < (tations)f(at)h(a)g(constan)n(t)g(pressure)f(of)h(1)g(atm)-150
12468 < 5277 y(for)d(50)f(ps)i(at)f(25)g(K.)g(Finally)-7 b(,)32
12469 < b(all)f(constrain)n(ts)g(w)n(ere)f(remo)n(v)n(ed)-150
12470 < 5372 y(and)d(the)g(ice)g(crystals)e(w)n(ere)h(allo)n(w)n(ed)f(to)i
12471 < (equilibrate)f(for)h(50)e(ps)2055 -166 y
12475 > (e)h(with)-150 5277 y(a)43 b(edge)g(length)h(ratio)e(of)i(appro)n
12476 > (ximately)d(1.00)p Ff(\002)p Fu(1.06)p Ff(\002)p Fu(1.23.)-150
12477 > 5372 y(The)e(particles)e(w)n(ere)h(then)h(allo)n(w)n(ed)e(to)i(orien)n
12478 > (t)e(freely)h(ab)r(out)2055 -166 y
12479   gsave currentpoint currentpoint translate -90 neg rotate neg exch
12480   neg exch translate
12481 < 2055 -166 a
12482 < @beginspecial 96 @llx 70 @lly 546 @urx 661 @ury 1842
12476 < @rwi @setspecial
12481 > 2055 -166 a @beginspecial
12482 > 96 @llx 70 @lly 546 @urx 661 @ury 1842 @rwi @setspecial
12483   %%BeginDocument: 1hdense.epsi
12484   %!PS-Adobe-2.0 EPSF-1.2
12485   %%Title: 1hdense.ps
# Line 20863 | Line 20869 | cleartomark countdictstack exch sub { end } repeat res
20869   %%EndDocument
20870   @endspecial 3590 -166 a
20871   currentpoint grestore moveto
20872 < 3590 -166 a 2042 1513 a Fq(FIG.)j(2:)38
20873 < b(Av)n(erage)28 b(densit)n(y)e(of)j(SSD)d(w)n(ater)i(at)g(increasing)h
20874 < (temp)r(er-)2042 1600 y(atures)d(starting)g(from)g(ice)g
20875 < Fp(I)2890 1609 y Fo(h)2955 1600 y Fq(lattice.)2042 1880
20876 < y Ft(at)32 b(25)g(K)h(and)g(a)f(constan)n(t)g(pressure)g(of)g(1)h(atm.)
20877 < 52 b(This)33 b(pro)r(ce-)2042 1975 y(dure)i(resulted)g(in)h
20878 < (structurally)f(stable)g Fi(I)3409 1987 y Fh(h)3488 1975
20879 < y Ft(ice)h(crystals)e(that)2042 2071 y(ob)r(ey)26 b(the)g(Bernal-F)-7
20880 < b(o)n(wler)24 b(rules)3084 2041 y Fm(16,17)3239 2071
20881 < y Ft(.)36 b(This)26 b(metho)r(d)h(w)n(as)e(also)2042
20882 < 2166 y(utilized)j(in)h(the)f(making)f(of)h(diamond)g(lattice)g
20883 < Fi(I)3598 2178 y Fh(c)3661 2166 y Ft(ice)f(crystals,)2042
20884 < 2262 y(with)22 b(eac)n(h)f(cubic)h(sim)n(ulation)f(b)r(o)n(x)g
20885 < (consisting)g(of)g(either)h(512)e(or)2042 2357 y(1000)30
20872 > 3590 -166 a 2042 1513 a Fr(FIG.)28
20873 > b(2:)38 b(Av)n(erage)28 b(densit)n(y)e(of)j(SSD)d(w)n(ater)i(at)g
20874 > (increasing)h(temp)r(er-)2042 1600 y(atures)d(starting)g(from)g(ice)g
20875 > Fq(I)2890 1609 y Fp(h)2955 1600 y Fr(lattice.)2042 1880
20876 > y Fu(\014xed)d(p)r(ositions)f(with)i(angular)d(momen)n(ta)i(randomized)
20877 > f(at)h(400)2042 1975 y(K)40 b(for)g(v)-5 b(arying)39
20878 > b(times.)75 b(The)40 b(rotational)f(temp)r(erature)h(w)n(as)2042
20879 > 2071 y(then)f(scaled)g(do)n(wn)g(in)g(stages)f(to)h(slo)n(wly)f(co)r
20880 > (ol)h(the)h(crystals)2042 2166 y(do)n(wn)27 b(to)g(25)f(K.)h(The)h
20881 > (particles)e(w)n(ere)g(then)i(allo)n(w)n(ed)e(translate)2042
20882 > 2262 y(with)35 b(\014xed)f(orien)n(tations)f(at)h(a)g(constan)n(t)g
20883 > (pressure)f(of)h(1)g(atm)2042 2357 y(for)d(50)f(ps)i(at)f(25)f(K.)i
20884 > (Finally)-7 b(,)32 b(all)f(constrain)n(ts)f(w)n(ere)h(remo)n(v)n(ed)
20885 > 2042 2453 y(and)26 b(the)i(ice)e(crystals)g(w)n(ere)g(allo)n(w)n(ed)f
20886 > (to)i(equilibrate)f(for)g(50)g(ps)2042 2548 y(at)32 b(25)g(K)h(and)g(a)
20887 > f(constan)n(t)g(pressure)g(of)g(1)h(atm.)52 b(This)33
20888 > b(pro)r(ce-)2042 2644 y(dure)i(resulted)g(in)h(structurally)f(stable)g
20889 > Fj(I)3409 2656 y Fi(h)3488 2644 y Fu(ice)h(crystals)e(that)2042
20890 > 2739 y(ob)r(ey)26 b(the)g(Bernal-F)-7 b(o)n(wler)24 b(rules)3084
20891 > 2709 y Fn(17,18)3239 2739 y Fu(.)36 b(This)26 b(metho)r(d)h(w)n(as)e
20892 > (also)2042 2835 y(utilized)j(in)h(the)f(making)f(of)h(diamond)g
20893 > (lattice)g Fj(I)3598 2847 y Fi(c)3661 2835 y Fu(ice)f(crystals,)2042
20894 > 2930 y(with)22 b(eac)n(h)f(cubic)h(sim)n(ulation)f(b)r(o)n(x)g
20895 > (consisting)g(of)g(either)h(512)e(or)2042 3026 y(1000)30
20896   b(particles.)51 b(Only)32 b(isotropic)f(v)n(olume)h(\015uctuations)g(w)
20897 < n(ere)2042 2453 y(p)r(erformed)e(under)h(constan)n(t)f(pressure,)h(so)f
20898 < (the)i(ratio)e(of)h(edge)2042 2548 y(lengths)c(remained)g(constan)n(t)g
20899 < (throughout)g(the)h(sim)n(ulations.)2349 2824 y Fn(I)r(I)r(I.)90
20900 < b(RESUL)-7 b(TS)29 b(AND)g(DISCUSSION)2125 3038 y Ft(Melting)c(studies)
20897 > n(ere)2042 3121 y(p)r(erformed)e(under)h(constan)n(t)f(pressure,)h(so)f
20898 > (the)i(ratio)e(of)h(edge)2042 3217 y(lengths)c(remained)g(constan)n(t)g
20899 > (throughout)g(the)h(sim)n(ulations.)2349 3493 y Fo(I)r(I)r(I.)90
20900 > b(RESUL)-7 b(TS)29 b(AND)g(DISCUSSION)2125 3706 y Fu(Melting)c(studies)
20901   g(w)n(ere)g(p)r(erformed)f(on)h(the)h(randomized)e(ice)2042
20902 < 3134 y(crystals)18 b(using)i(constan)n(t)f(pressure)f(and)i(temp)r
20903 < (erature)g(dynam-)2042 3229 y(ics.)84 b(This)44 b(in)n(v)n(olv)n(ed)e
20902 > 3802 y(crystals)18 b(using)i(constan)n(t)f(pressure)f(and)i(temp)r
20903 > (erature)g(dynam-)2042 3897 y(ics.)84 b(This)44 b(in)n(v)n(olv)n(ed)e
20904   (an)h(initial)h(randomization)e(of)h(v)n(elo)r(ci-)2042
20905 < 3324 y(ties)d(ab)r(out)h(the)g(starting)f(temp)r(erature)g(of)g(25)g(K)
20906 < g(for)g(v)-5 b(ary-)2042 3420 y(ing)31 b(amoun)n(ts)f(of)h(time.)49
20907 < b(The)31 b(systems)f(w)n(ere)h(all)g(equilibrated)2042
20908 < 3515 y(for)g(100)g(ps)h(prior)f(to)g(a)h(200)f(ps)g(data)h(collection)f
20909 < (run)h(at)g(eac)n(h)2042 3611 y(temp)r(erature)i(setting,)j(ranging)c
20910 < (from)i(25)f(to)g(400)g(K,)g(with)i(a)2042 3706 y(maxim)n(um)f(degree)f
20911 < (incremen)n(t)h(of)g(25)f(K.)h(F)-7 b(or)35 b(regions)e(of)i(in-)2042
20912 < 3802 y(terest)h(along)f(this)i(step)n(wise)f(progression,)g(the)h(temp)
20913 < r(erature)2042 3897 y(incremen)n(t)i(w)n(as)g(decreased)f(from)h(25)g
20914 < (K)g(to)g(10)g(and)h(then)g(5)2042 3993 y(K.)26 b(The)g(a)n(v)n(erage)e
20915 < (densit)n(y)i(w)n(as)f(calculated)h(o)n(v)n(er)f(\014v)n(e)h(separate)
20916 < 2042 4088 y(sim)n(ulations)g(of)i Fi(I)2609 4100 y Fh(h)2679
20917 < 4088 y Ft(ice,)g(and)f(the)h(results)e(are)h(sho)n(wn)f(in)i(\014gure)
20918 < 2042 4184 y(2.)2638 4460 y Fn(A.)88 b(Densit)n(y)29 b(Beha)n(vior)2125
20919 < 4673 y Ft(In)e(the)h(initial)g(a)n(v)n(erage)d(densit)n(y)i(v)n(ersus)f
20920 < (temp)r(erature)h(plot,)2042 4769 y(the)34 b(densit)n(y)g(maxim)n(um)g
20921 < (clearly)f(app)r(ears)g(b)r(et)n(w)n(een)i(255)d(and)2042
20922 < 4864 y(265)i(K.)h(The)h(calculated)f(densities)h(within)g(this)g(range)
20923 < e(w)n(ere)2042 4960 y(nearly)f(indistinguishable,)i(as)e(can)g(b)r(e)h
20924 < (seen)g(in)g(the)g(zo)r(om)f(of)2042 5055 y(this)k(region)f(of)i(in)n
20925 < (terest,)h(sho)n(wn)e(in)g(\014gure)g(2.)66 b(The)37
20910 < b(greater)2042 5151 y(certain)n(t)n(y)24 b(of)h(the)h(a)n(v)n(erage)c
20911 < (v)-5 b(alue)26 b(at)f(260)f(K)h(mak)n(es)f(a)h(go)r(o)r(d)f(ar-)2042
20912 < 5246 y(gumen)n(t)k(for)g(the)h(actual)f(densit)n(y)g(maxim)n(um)g
20913 < (residing)g(at)g(this)2042 5342 y(midp)r(oin)n(t)36 b(v)-5
20914 < b(alue.)61 b(Figure)35 b(2)g(w)n(as)g(constructed)g(using)g(ice)h
20915 < Fi(I)4041 5354 y Fh(h)p eop
20905 > 3993 y(ties)31 b(ab)r(out)h(the)f(starting)g(temp)r(erature)g(of)g(25)g
20906 > (K)g(for)f(v)-5 b(arying)2042 4088 y(amoun)n(ts)31 b(of)i(time.)51
20907 > b(The)33 b(systems)e(w)n(ere)h(all)g(equilibrated)g(for)2042
20908 > 4184 y(100)25 b(ps)h(prior)f(to)i(a)f(200)f(ps)h(data)g(collection)g
20909 > (run)g(at)g(eac)n(h)g(tem-)2042 4279 y(p)r(erature)g(setting,)h
20910 > (ranging)f(from)h(25)f(to)h(400)f(K,)h(with)g(a)g(max-)2042
20911 > 4375 y(im)n(um)33 b(degree)f(incremen)n(t)h(of)g(25)f(K.)h(F)-7
20912 > b(or)32 b(regions)g(of)h(in)n(terest)2042 4470 y(along)i(this)i(step)n
20913 > (wise)f(progression,)g(the)h(temp)r(erature)f(incre-)2042
20914 > 4566 y(men)n(t)28 b(w)n(as)g(decreased)f(from)h(25)f(K)h(to)h(10)e(and)
20915 > h(then)h(5)f(K.)g(The)2042 4661 y(ab)r(o)n(v)n(e)e(equilibration)i(and)
20916 > f(pro)r(duction)h(times)g(w)n(ere)f(su\016cien)n(t)2042
20917 > 4757 y(in)g(that)g(the)g(system)f(v)n(olume)g(\015uctuations)h(damp)r
20918 > (ened)g(out)g(in)2042 4852 y(all)34 b(but)g(the)h(v)n(ery)e(cold)g(sim)
20919 > n(ulations)g(\(b)r(elo)n(w)h(225)f(K\).)h(In)g(or-)2042
20920 > 4948 y(der)23 b(to)h(further)g(impro)n(v)n(e)e(statistics,)j(\014v)n(e)
20921 > e(separate)g(sim)n(ulation)2042 5043 y(progressions)37
20922 > b(w)n(ere)i(p)r(erformed,)k(and)d(the)g(a)n(v)n(eraged)e(results)2042
20923 > 5138 y(from)27 b(the)h Fj(I)2417 5150 y Fi(h)2488 5138
20924 > y Fu(melting)g(sim)n(ulations)f(are)f(sho)n(wn)h(in)h(\014gure)f(2.)p
20925 > eop
20926   %%Page: 4 4
20927 < 4 3 bop 4043 -299 a Ft(4)-150 -166 y
20927 > 4 3 bop 4043 -299 a Fu(4)-150 -166 y
20928   gsave currentpoint currentpoint translate -90 neg rotate neg exch
20929   neg exch translate
20930   -150 -166 a @beginspecial
# Line 30036 | Line 30046 | userdict /ai9_skip_data get exec
30046   %%EndDocument
30047   @endspecial 1385 -166 a
30048   currentpoint grestore moveto
30049 < 1385 -166 a -150 1525 a Fq(FIG.)81
30049 > 1385 -166 a -150 1525 a Fr(FIG.)81
30050   b(3:)144 b(Densit)n(y)80 b(v)n(ersus)g(temp)r(erature)g(for)h(TIP4P)
30051 < 1805 1493 y Fc(18)1871 1525 y Fq(,)-150 1612 y(TIP3P)75
30052 < 1580 y Fc(18)141 1612 y Fq(,)33 b(SPC/E)435 1580 y Fc(19)501
30053 < 1612 y Fq(,)g(SSD)d(without)i(Reaction)f(Field,)j(SSD,)d(and)-150
30054 < 1699 y(Exp)r(erimen)n(t)243 1667 y Fc(20)307 1699 y Fq(.)-150
30055 < 1979 y Ft(crystals)24 b(for)g(the)h(initial)g(con\014guration;)f(and)h
30056 < (though)g(not)g(pic-)-150 2075 y(tured,)h(the)f(sim)n(ulations)f
30057 < (starting)g(from)h(ice)f Fi(I)1325 2087 y Fh(c)1385 2075
30058 < y Ft(crystal)f(con\014g-)-150 2170 y(urations)j(sho)n(w)n(ed)f(similar)
30059 < h(results,)g(with)h(a)g(liquid-phase)f(den-)-150 2266
30060 < y(sit)n(y)g(maxim)n(um)h(in)f(this)h(same)f(region)f(\(b)r(et)n(w)n
30061 < (een)i(255)e(and)i(260)-150 2361 y(K\).)f(In)h(addition,)g(the)g
30062 < Fi(I)627 2373 y Fh(c)688 2361 y Ft(crystals)e(are)g(more)h(fragile)f
30063 < (than)i(the)-150 2456 y Fi(I)-114 2468 y Fh(h)-37 2456
30064 < y Ft(crystals,)33 b(leading)f(them)i(to)f(deform)g(in)n(to)f(a)h(dense)
30065 < g(glassy)-150 2552 y(state)d(at)h(lo)n(w)n(er)d(temp)r(eratures.)45
30066 < b(This)31 b(resulted)f(in)g(an)h(o)n(v)n(erall)-150 2647
30067 < y(lo)n(w)k(temp)r(erature)g(densit)n(y)h(maxim)n(um)g(at)f(200)f(K,)i
30068 < (but)g(they)-150 2743 y(still)i(retained)g(a)g(common)f(liquid)i(state)
30069 < f(densit)n(y)g(maxim)n(um)-150 2838 y(with)28 b(the)g
30070 < Fi(I)218 2850 y Fh(h)289 2838 y Ft(sim)n(ulations.)-67
30071 < 2934 y(The)19 b(densit)n(y)g(maxim)n(um)g(for)g(SSD)h(actually)e
30072 < (compares)g(quite)-150 3029 y(fa)n(v)n(orably)h(to)j(other)f(simple)h
30073 < (w)n(ater)f(mo)r(dels.)35 b(Figure)21 b(3)g(sho)n(ws)g(a)-150
30074 < 3125 y(plot)j(of)g(these)f(\014ndings)h(with)g(the)h(densit)n(y)e
30075 < (progression)e(of)j(sev-)-150 3220 y(eral)36 b(other)g(mo)r(dels)h(and)
30076 < f(exp)r(erimen)n(t)h(obtained)g(from)f(other)-150 3316
30077 < y(sources.)134 3286 y Fm(18)o({20)328 3316 y Ft(Of)26
30051 > 1805 1493 y Fc(19)1871 1525 y Fr(,)-150 1612 y(TIP3P)75
30052 > 1580 y Fc(19)141 1612 y Fr(,)33 b(SPC/E)435 1580 y Fc(20)501
30053 > 1612 y Fr(,)g(SSD)d(without)i(Reaction)f(Field,)j(SSD,)d(and)-150
30054 > 1699 y(Exp)r(erimen)n(t)243 1667 y Fc(21)307 1699 y Fr(.)446
30055 > 1979 y Fo(A.)88 b(Densit)n(y)29 b(Beha)n(vior)-67 2193
30056 > y Fu(In)f(the)g(initial)f(a)n(v)n(erage)e(densit)n(y)i(v)n(ersus)f
30057 > (temp)r(erature)h(plot,)-150 2288 y(the)35 b(densit)n(y)f(maxim)n(um)g
30058 > (clearly)f(app)r(ears)g(b)r(et)n(w)n(een)h(255)f(and)-150
30059 > 2384 y(265)h(K.)i(The)f(calculated)g(densities)h(within)g(this)g(range)
30060 > e(w)n(ere)-150 2479 y(nearly)f(indistinguishable,)i(as)e(can)g(b)r(e)i
30061 > (seen)e(in)h(the)g(zo)r(om)f(of)-150 2575 y(this)38 b(region)e(of)h(in)
30062 > n(terest,)i(sho)n(wn)e(in)h(\014gure)e(2.)66 b(The)37
30063 > b(greater)-150 2670 y(certain)n(t)n(y)24 b(of)h(the)h(a)n(v)n(erage)d
30064 > (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
30065 > 2766 y(gumen)n(t)j(for)g(the)h(actual)f(densit)n(y)g(maxim)n(um)g
30066 > (residing)g(at)g(this)-150 2861 y(midp)r(oin)n(t)36 b(v)-5
30067 > b(alue.)61 b(Figure)35 b(2)g(w)n(as)g(constructed)g(using)g(ice)h
30068 > Fj(I)1849 2873 y Fi(h)-150 2956 y Fu(crystals)24 b(for)g(the)h(initial)
30069 > g(con\014guration;)f(and)h(though)g(not)g(pic-)-150 3052
30070 > y(tured,)h(the)f(sim)n(ulations)f(starting)g(from)h(ice)f
30071 > Fj(I)1325 3064 y Fi(c)1385 3052 y Fu(crystal)f(con\014g-)-150
30072 > 3147 y(urations)j(sho)n(w)n(ed)f(similar)h(results,)g(with)h(a)g
30073 > (liquid-phase)f(den-)-150 3243 y(sit)n(y)g(maxim)n(um)h(in)f(this)h
30074 > (same)f(region)f(\(b)r(et)n(w)n(een)i(255)e(and)i(260)-150
30075 > 3338 y(K\).)f(In)h(addition,)g(the)g Fj(I)627 3350 y
30076 > Fi(c)688 3338 y Fu(crystals)e(are)g(more)h(fragile)f(than)i(the)-150
30077 > 3434 y Fj(I)-114 3446 y Fi(h)-37 3434 y Fu(crystals,)33
30078 > b(leading)f(them)i(to)f(deform)g(in)n(to)f(a)h(dense)g(glassy)-150
30079 > 3529 y(state)d(at)h(lo)n(w)n(er)d(temp)r(eratures.)45
30080 > b(This)31 b(resulted)f(in)g(an)h(o)n(v)n(erall)-150 3625
30081 > y(lo)n(w)k(temp)r(erature)g(densit)n(y)h(maxim)n(um)g(at)f(200)f(K,)i
30082 > (but)g(they)-150 3720 y(still)i(retained)g(a)g(common)f(liquid)i(state)
30083 > f(densit)n(y)g(maxim)n(um)-150 3816 y(with)28 b(the)g
30084 > Fj(I)218 3828 y Fi(h)289 3816 y Fu(sim)n(ulations.)-67
30085 > 3911 y(The)19 b(densit)n(y)g(maxim)n(um)g(for)g(SSD)h(actually)e
30086 > (compares)g(quite)-150 4007 y(fa)n(v)n(orably)h(to)j(other)f(simple)h
30087 > (w)n(ater)f(mo)r(dels.)35 b(Figure)21 b(3)g(sho)n(ws)g(a)-150
30088 > 4102 y(plot)j(of)g(these)f(\014ndings)h(with)g(the)h(densit)n(y)e
30089 > (progression)e(of)j(sev-)-150 4198 y(eral)36 b(other)g(mo)r(dels)h(and)
30090 > f(exp)r(erimen)n(t)h(obtained)g(from)f(other)-150 4293
30091 > y(sources.)134 4263 y Fn(19)o({21)328 4293 y Fu(Of)26
30092   b(the)g(listed)g(simple)g(w)n(ater)f(mo)r(dels,)h(SSD)h(has)-150
30093 < 3411 y(results)d(closest)g(to)h(the)g(exp)r(erimen)n(tally)f(observ)n
30094 < (ed)f(w)n(ater)h(den-)-150 3507 y(sit)n(y)i(maxim)n(um.)36
30093 > 4389 y(results)d(closest)g(to)h(the)g(exp)r(erimen)n(tally)f(observ)n
30094 > (ed)f(w)n(ater)h(den-)-150 4484 y(sit)n(y)i(maxim)n(um.)36
30095   b(Of)27 b(the)g(listed)f(w)n(ater)f(mo)r(dels,)i(TIP4P)e(has)h(a)-150
30096 < 3602 y(densit)n(y)32 b(maxim)n(um)g(b)r(eha)n(vior)f(most)h(lik)n(e)g
30097 < (that)h(seen)f(in)h(SSD.)-150 3698 y(Though)f(not)g(sho)n(wn,)h(it)f
30098 < (is)h(useful)f(to)g(note)h(that)f(TIP5P)f(has)-150 3793
30099 < y(a)j(w)n(ater)f(densit)n(y)h(maxim)n(um)g(nearly)f(iden)n(tical)h
30100 < (with)h(exp)r(eri-)-150 3889 y(men)n(t.)-67 3984 y(P)n(ossibly)c(of)i
30101 < (more)g(imp)r(ortance)f(is)h(the)h(densit)n(y)e(scaling)g(of)-150
30102 < 4080 y(SSD)27 b(relativ)n(e)f(to)h(other)f(common)g(mo)r(dels)h(at)f
30103 < (an)n(y)g(giv)n(en)g(tem-)-150 4175 y(p)r(erature)31
30104 < b(\(Fig.)48 b(3\).)f(Note)32 b(that)f(the)h(SSD)g(mo)r(del)g(assumes)e
30105 < (a)-150 4271 y(lo)n(w)n(er)e(densit)n(y)h(than)g(an)n(y)f(of)h(the)h
30106 < (other)e(listed)i(mo)r(dels)f(at)g(the)-150 4366 y(same)i(pressure,)h
30107 < (b)r(eha)n(vior)e(whic)n(h)i(is)g(esp)r(ecially)f(apparen)n(t)g(at)-150
30108 < 4461 y(temp)r(eratures)h(greater)f(than)i(300)e(K.)h(Lo)n(w)n(er)f
30109 < (than)i(exp)r(ected)-150 4557 y(densities)d(ha)n(v)n(e)f(b)r(een)h
30110 < (observ)n(ed)e(for)i(other)f(systems)h(with)g(the)-150
30111 < 4652 y(use)j(of)f(a)g(reaction)g(\014eld)h(for)f(long-range)e
30112 < (electrostatic)i(in)n(ter-)-150 4748 y(actions,)h(so)e(the)i(most)e
30113 < (lik)n(ely)h(reason)f(for)g(these)h(signi\014can)n(tly)-150
30114 < 4843 y(lo)n(w)n(er)23 b(densities)h(in)h(these)g(sim)n(ulations)f(is)g
30115 < (the)h(presence)f(of)g(the)-150 4939 y(reaction)36 b(\014eld.)353
30116 < 4909 y Fm(11)460 4939 y Ft(In)h(order)e(to)i(test)g(the)g(e\013ect)g
30117 < (of)g(the)g(reac-)-150 5034 y(tion)30 b(\014eld)h(on)f(the)h(densit)n
30118 < (y)f(of)h(the)g(systems,)f(the)h(sim)n(ulations)-150
30119 < 5130 y(w)n(ere)19 b(rep)r(eated)g(for)g(the)h(temp)r(erature)g(region)e
30120 < (of)i(in)n(terest)f(with-)-150 5225 y(out)34 b(a)f(reaction)g(\014eld)h
30121 < (presen)n(t.)54 b(The)34 b(results)f(of)h(these)g(sim)n(u-)-150
30122 < 5321 y(lations)e(are)g(also)g(displa)n(y)n(ed)g(in)h(\014gure)f(3.)52
30123 < b(Without)34 b(reaction)2042 -83 y(\014eld,)27 b(these)g(densities)f
30124 < (increase)g(considerably)f(to)i(m)n(uc)n(h)f(more)2042
30125 < 12 y(exp)r(erimen)n(tally)33 b(reasonable)e(v)-5 b(alues,)35
30126 < b(esp)r(ecially)e(around)g(the)2042 108 y(freezing)i(p)r(oin)n(t)i(of)f
30127 < (liquid)g(w)n(ater.)62 b(The)36 b(shap)r(e)g(of)h(the)f(curv)n(e)2042
30128 < 203 y(is)g(similar)f(to)h(the)h(curv)n(e)e(pro)r(duced)h(from)g(SSD)h
30129 < (sim)n(ulations)2042 299 y(using)j(reaction)g(\014eld,)k(sp)r
30130 < (eci\014cally)d(the)g(rapidly)f(decreasing)2042 394 y(densities)31
30131 < b(at)g(higher)f(temp)r(eratures;)i(ho)n(w)n(ev)n(er,)e(a)g(sligh)n(t)h
30132 < (shift)2042 490 y(in)d(the)g(densit)n(y)g(maxim)n(um)g(lo)r(cation,)f
30133 < (do)n(wn)g(to)h(245)e(K,)i(is)g(ob-)2042 585 y(serv)n(ed.)39
30134 < b(This)29 b(is)g(probably)e(a)i(more)f(accurate)f(comparison)g(to)2042
30135 < 681 y(the)i(other)g(listed)g(w)n(ater)f(mo)r(dels)i(in)f(that)g(no)g
30136 < (long)g(range)f(cor-)2042 776 y(rections)e(w)n(ere)h(applied)h(in)g
30137 < (those)f(sim)n(ulations.)3581 746 y Fm(18)o(,19)2125
30138 < 872 y Ft(It)33 b(has)e(b)r(een)i(observ)n(ed)e(that)i(densities)f(are)f
30139 < (dep)r(enden)n(t)i(on)2042 967 y(the)j(cuto\013)h(radius)e(used)h(for)f
30140 < (a)h(v)-5 b(ariet)n(y)35 b(of)h(w)n(ater)f(mo)r(dels)h(in)2042
30141 < 1063 y(sim)n(ulations)g(b)r(oth)i(with)g(and)f(without)h(the)g(use)f
30142 < (of)g(reaction)2042 1158 y(\014eld.)2217 1128 y Fm(11)2323
30143 < 1158 y Ft(In)f(order)e(to)h(address)g(the)h(p)r(ossible)f(a\013ect)g
30144 < (of)h(cuto\013)2042 1254 y(radius,)26 b(sim)n(ulations)g(w)n(ere)h(p)r
30145 < (erformed)f(with)i(a)e(dip)r(olar)h(cuto\013)2042 1349
30146 < y(radius)j(of)g(12.0)2571 1334 y(\027)2571 1349 y(A)h(to)g(complimen)n
30147 < (t)f(the)i(previous)d(SSD)j(sim)n(u-)2042 1445 y(lations,)e(all)g(p)r
30148 < (erformed)g(with)h(a)f(cuto\013)g(of)g(9.0)3587 1430
30149 < y(\027)3587 1445 y(A.)h(All)f(the)h(re-)2042 1540 y(sulting)e
30150 < (densities)h(o)n(v)n(erlapp)r(ed)e(within)j(error)c(and)j(sho)n(w)n(ed)
30151 < e(no)2042 1636 y(signi\014can)n(t)21 b(trend)h(in)g(lo)n(w)n(er)f(or)g
30152 < (higher)g(densities)i(as)e(a)h(function)2042 1731 y(of)33
30153 < b(cuto\013)h(radius,)h(b)r(oth)f(for)f(sim)n(ulations)g(with)h(and)g
30154 < (without)2042 1826 y(reaction)39 b(\014eld.)77 b(These)40
30155 < b(results)g(indicate)h(that)g(there)f(is)g(no)2042 1922
30156 < y(ma)5 b(jor)26 b(b)r(ene\014t)i(in)f(c)n(ho)r(osing)f(a)h(longer)f
30157 < (cuto\013)i(radius)e(in)i(sim)n(u-)2042 2017 y(lations)23
30158 < b(using)h(SSD.)h(This)f(is)g(comforting)f(in)h(that)g(the)h(use)f(of)g
30159 < (a)2042 2113 y(longer)e(cuto\013)h(radius)f(results)h(in)g(a)g(near)f
30160 < (doubling)h(of)g(the)h(time)2042 2208 y(required)i(to)i(compute)g(a)f
30161 < (single)g(tra)5 b(jectory)-7 b(.)2596 2485 y Fn(B.)88
30162 < b(T)-7 b(ransp)r(ort)30 b(Beha)n(vior)2125 2698 y Ft(Of)f(imp)r
30163 < (ortance)f(in)h(these)f(t)n(yp)r(es)h(of)g(studies)f(are)g(the)h
30164 < (trans-)2042 2794 y(p)r(ort)44 b(prop)r(erties)f(of)h(the)g(particles)f
30165 < (and)h(ho)n(w)f(they)h(c)n(hange)2042 2889 y(when)29
30166 < b(altering)f(the)h(en)n(vironmen)n(tal)e(conditions.)41
30167 < b(In)29 b(order)e(to)2042 2985 y(prob)r(e)34 b(transp)r(ort,)i(constan)
30168 < n(t)d(energy)h(sim)n(ulations)g(w)n(ere)g(p)r(er-)2042
30169 < 3080 y(formed)27 b(ab)r(out)g(the)h(a)n(v)n(erage)c(densit)n(y)j(unco)n
30170 < (v)n(ered)f(b)n(y)h(the)h(con-)2042 3175 y(stan)n(t)21
30171 < b(pressure)g(sim)n(ulations.)34 b(Sim)n(ulations)22 b(started)f(with)h
30172 < (ran-)2042 3271 y(domized)32 b(v)n(elo)r(cities)f(and)h(underw)n(en)n
30173 < (t)g(50)f(ps)h(of)h(temp)r(erature)2042 3366 y(scaling)25
30174 < b(and)h(50)f(ps)h(of)g(constan)n(t)f(energy)g(equilibration)g(b)r
30175 < (efore)2042 3462 y(obtaining)32 b(a)h(200)e(ps)i(tra)5
30176 < b(jectory)-7 b(.)52 b(Di\013usion)33 b(constan)n(ts)f(w)n(ere)2042
30177 < 3557 y(calculated)27 b(via)h(ro)r(ot-mean)f(square)f(deviation)i
30178 < (analysis.)37 b(The)2042 3653 y(a)n(v)n(eraged)e(results)i(from)h(5)f
30179 < (sets)h(of)f(these)h(NVE)g(sim)n(ulations)2042 3748 y(is)29
30180 < b(displa)n(y)n(ed)f(in)i(\014gure)f(4,)g(alongside)f(exp)r(erimen)n
30181 < (tal,)h(SPC/E,)2042 3844 y(and)e(TIP5P)f(results.)2735
30182 < 3814 y Fm(4,19,21,22)2125 3939 y Ft(The)38 b(observ)n(ed)e(v)-5
30183 < b(alues)37 b(for)g(the)h(di\013usion)g(constan)n(t)f(p)r(oin)n(t)2042
30184 < 4035 y(out)45 b(one)g(of)g(the)h(strengths)e(of)h(the)h(SSD)g(mo)r
30185 < (del.)90 b(Of)45 b(the)2042 4130 y(three)39 b(exp)r(erimen)n(tal)g(mo)r
30186 < (dels)g(sho)n(wn,)j(the)e(SSD)g(mo)r(del)g(has)2042 4226
30187 < y(the)23 b(most)g(accurate)f(depiction)i(of)f(the)g(di\013usion)h
30188 < (trend)f(seen)g(in)2042 4321 y(exp)r(erimen)n(t)i(in)g(b)r(oth)h(the)g
30189 < (sup)r(erco)r(oled)e(and)h(normal)f(regimes.)2042 4417
30096 > 4580 y(densit)n(y)32 b(maxim)n(um)g(b)r(eha)n(vior)f(most)h(lik)n(e)g
30097 > (that)h(seen)f(in)h(SSD.)-150 4675 y(Though)25 b(not)h(sho)n(wn,)f(it)h
30098 > (is)g(useful)g(to)f(note)h(that)g(TIP5P)e(has)h(a)-150
30099 > 4771 y(w)n(ater)i(densit)n(y)g(maxim)n(um)g(nearly)g(iden)n(tical)g(to)
30100 > h(exp)r(erimen)n(t.)-67 4866 y(P)n(ossibly)j(of)i(more)g(imp)r(ortance)
30101 > f(is)h(the)h(densit)n(y)e(scaling)g(of)-150 4961 y(SSD)27
30102 > b(relativ)n(e)f(to)h(other)f(common)g(mo)r(dels)h(at)f(an)n(y)g(giv)n
30103 > (en)g(tem-)-150 5057 y(p)r(erature)31 b(\(Fig.)48 b(3\).)f(Note)32
30104 > b(that)f(the)h(SSD)g(mo)r(del)g(assumes)e(a)-150 5152
30105 > y(lo)n(w)n(er)e(densit)n(y)h(than)g(an)n(y)f(of)h(the)h(other)e(listed)
30106 > i(mo)r(dels)f(at)g(the)-150 5248 y(same)i(pressure,)h(b)r(eha)n(vior)e
30107 > (whic)n(h)i(is)g(esp)r(ecially)f(apparen)n(t)g(at)-150
30108 > 5343 y(temp)r(eratures)h(greater)f(than)i(300)e(K.)h(Lo)n(w)n(er)f
30109 > (than)i(exp)r(ected)2042 -83 y(densities)d(ha)n(v)n(e)e(b)r(een)j
30110 > (observ)n(ed)d(for)i(other)f(systems)g(with)i(the)2042
30111 > 12 y(use)h(of)h(a)f(reaction)g(\014eld)h(for)f(long-range)e
30112 > (electrostatic)i(in)n(ter-)2042 108 y(actions,)g(so)g(the)g(most)g(lik)
30113 > n(ely)g(reason)e(for)i(these)g(signi\014can)n(tly)2042
30114 > 203 y(lo)n(w)n(er)23 b(densities)h(in)h(these)g(sim)n(ulations)e(is)i
30115 > (the)g(presence)e(of)i(the)2042 299 y(reaction)f(\014eld.)2533
30116 > 269 y Fn(12)2629 299 y Fu(In)h(order)f(to)h(test)g(the)h(e\013ect)g(of)
30117 > f(the)g(reaction)2042 394 y(\014eld)j(on)g(the)h(densit)n(y)f(of)g(the)
30118 > g(systems,)g(the)h(sim)n(ulations)e(w)n(ere)2042 490
30119 > y(rep)r(eated)32 b(for)g(the)i(temp)r(erature)e(region)g(of)g(in)n
30120 > (terest)h(without)2042 585 y(a)27 b(reaction)g(\014eld)h(presen)n(t.)37
30121 > b(The)28 b(results)f(of)h(these)g(sim)n(ulations)2042
30122 > 681 y(are)38 b(also)g(displa)n(y)n(ed)h(in)g(\014gure)g(3.)71
30123 > b(Without)41 b(reaction)d(\014eld,)2042 776 y(these)26
30124 > b(densities)f(increase)g(considerably)f(to)i(more)f(exp)r(erimen-)2042
30125 > 872 y(tally)43 b(reasonable)e(v)-5 b(alues,)46 b(esp)r(ecially)d
30126 > (around)e(the)j(freezing)2042 967 y(p)r(oin)n(t)37 b(of)g(liquid)h(w)n
30127 > (ater.)64 b(The)38 b(shap)r(e)e(of)i(the)f(curv)n(e)f(is)h(simi-)2042
30128 > 1063 y(lar)g(to)h(the)g(curv)n(e)f(pro)r(duced)h(from)g(SSD)g(sim)n
30129 > (ulations)g(using)2042 1158 y(reaction)e(\014eld,)k(sp)r(eci\014cally)c
30130 > (the)i(rapidly)e(decreasing)f(densi-)2042 1254 y(ties)24
30131 > b(at)g(higher)g(temp)r(eratures;)g(ho)n(w)n(ev)n(er,)f(a)h(sligh)n(t)g
30132 > (shift)g(in)h(the)2042 1349 y(densit)n(y)30 b(maxim)n(um)g(lo)r
30133 > (cation,)g(do)n(wn)f(to)h(245)f(K,)h(is)g(observ)n(ed.)2042
30134 > 1445 y(This)21 b(is)f(probably)g(a)g(more)g(accurate)g(comparison)f(to)
30135 > i(the)g(other)2042 1540 y(listed)f(w)n(ater)f(mo)r(dels)g(in)h(that)g
30136 > (no)g(long)f(range)f(corrections)g(w)n(ere)2042 1636
30137 > y(applied)27 b(in)h(those)f(sim)n(ulations.)3079 1605
30138 > y Fn(19,20)2125 1731 y Fu(It)33 b(has)e(b)r(een)i(observ)n(ed)e(that)i
30139 > (densities)f(are)f(dep)r(enden)n(t)i(on)2042 1826 y(the)j(cuto\013)h
30140 > (radius)e(used)h(for)f(a)h(v)-5 b(ariet)n(y)35 b(of)h(w)n(ater)f(mo)r
30141 > (dels)h(in)2042 1922 y(sim)n(ulations)g(b)r(oth)i(with)g(and)f(without)
30142 > h(the)g(use)f(of)g(reaction)2042 2017 y(\014eld.)2217
30143 > 1987 y Fn(12)2323 2017 y Fu(In)f(order)e(to)h(address)g(the)h(p)r
30144 > (ossible)f(a\013ect)g(of)h(cuto\013)2042 2113 y(radius,)26
30145 > b(sim)n(ulations)g(w)n(ere)h(p)r(erformed)f(with)i(a)e(dip)r(olar)h
30146 > (cuto\013)2042 2208 y(radius)j(of)g(12.0)2571 2193 y(\027)2571
30147 > 2208 y(A)h(to)g(complimen)n(t)f(the)i(previous)d(SSD)j(sim)n(u-)2042
30148 > 2304 y(lations,)e(all)g(p)r(erformed)g(with)h(a)f(cuto\013)g(of)g(9.0)
30149 > 3587 2289 y(\027)3587 2304 y(A.)h(All)f(the)h(re-)2042
30150 > 2399 y(sulting)e(densities)h(o)n(v)n(erlapp)r(ed)e(within)j(error)c
30151 > (and)j(sho)n(w)n(ed)e(no)2042 2495 y(signi\014can)n(t)21
30152 > b(trend)h(in)g(lo)n(w)n(er)f(or)g(higher)g(densities)i(as)e(a)h
30153 > (function)2042 2590 y(of)33 b(cuto\013)h(radius,)h(b)r(oth)f(for)f(sim)
30154 > n(ulations)g(with)h(and)g(without)2042 2686 y(reaction)39
30155 > b(\014eld.)77 b(These)40 b(results)g(indicate)h(that)g(there)f(is)g(no)
30156 > 2042 2781 y(ma)5 b(jor)26 b(b)r(ene\014t)i(in)f(c)n(ho)r(osing)f(a)h
30157 > (longer)f(cuto\013)i(radius)e(in)i(sim)n(u-)2042 2877
30158 > y(lations)23 b(using)h(SSD.)h(This)f(is)g(comforting)f(in)h(that)g(the)
30159 > h(use)f(of)g(a)2042 2972 y(longer)e(cuto\013)h(radius)f(results)h(in)g
30160 > (a)g(near)f(doubling)h(of)g(the)h(time)2042 3068 y(required)i(to)i
30161 > (compute)g(a)f(single)g(tra)5 b(jectory)-7 b(.)2596 3344
30162 > y Fo(B.)88 b(T)-7 b(ransp)r(ort)30 b(Beha)n(vior)2125
30163 > 3557 y Fu(Of)f(imp)r(ortance)f(in)h(these)f(t)n(yp)r(es)h(of)g(studies)
30164 > f(are)g(the)h(trans-)2042 3653 y(p)r(ort)44 b(prop)r(erties)f(of)h(the)
30165 > g(particles)f(and)h(ho)n(w)f(they)h(c)n(hange)2042 3748
30166 > y(when)29 b(altering)f(the)h(en)n(vironmen)n(tal)e(conditions.)41
30167 > b(In)29 b(order)e(to)2042 3844 y(prob)r(e)34 b(transp)r(ort,)i(constan)
30168 > n(t)d(energy)h(sim)n(ulations)g(w)n(ere)g(p)r(er-)2042
30169 > 3939 y(formed)27 b(ab)r(out)g(the)h(a)n(v)n(erage)c(densit)n(y)j(unco)n
30170 > (v)n(ered)f(b)n(y)h(the)h(con-)2042 4035 y(stan)n(t)21
30171 > b(pressure)g(sim)n(ulations.)34 b(Sim)n(ulations)22 b(started)f(with)h
30172 > (ran-)2042 4130 y(domized)32 b(v)n(elo)r(cities)f(and)h(underw)n(en)n
30173 > (t)g(50)f(ps)h(of)h(temp)r(erature)2042 4226 y(scaling)25
30174 > b(and)h(50)f(ps)h(of)g(constan)n(t)f(energy)g(equilibration)g(b)r
30175 > (efore)2042 4321 y(obtaining)32 b(a)h(200)e(ps)i(tra)5
30176 > b(jectory)-7 b(.)52 b(Di\013usion)33 b(constan)n(ts)f(w)n(ere)2042
30177 > 4417 y(calculated)27 b(via)h(ro)r(ot-mean)f(square)f(deviation)i
30178 > (analysis.)37 b(The)2042 4512 y(a)n(v)n(eraged)e(results)i(from)h(5)f
30179 > (sets)h(of)f(these)h(NVE)g(sim)n(ulations)2042 4608 y(is)29
30180 > b(displa)n(y)n(ed)f(in)i(\014gure)f(4,)g(alongside)f(exp)r(erimen)n
30181 > (tal,)h(SPC/E,)2042 4703 y(and)e(TIP5P)f(results.)2735
30182 > 4673 y Fn(4,20,22,23)2125 4799 y Fu(The)38 b(observ)n(ed)e(v)-5
30183 > b(alues)37 b(for)g(the)h(di\013usion)g(constan)n(t)f(p)r(oin)n(t)2042
30184 > 4894 y(out)45 b(one)g(of)g(the)h(strengths)e(of)h(the)h(SSD)g(mo)r
30185 > (del.)90 b(Of)45 b(the)2042 4990 y(three)39 b(exp)r(erimen)n(tal)g(mo)r
30186 > (dels)g(sho)n(wn,)j(the)e(SSD)g(mo)r(del)g(has)2042 5085
30187 > y(the)23 b(most)g(accurate)f(depiction)i(of)f(the)g(di\013usion)h
30188 > (trend)f(seen)g(in)2042 5180 y(exp)r(erimen)n(t)i(in)g(b)r(oth)h(the)g
30189 > (sup)r(erco)r(oled)e(and)h(normal)f(regimes.)2042 5276
30190   y(SPC/E)19 b(do)r(es)h(a)g(resp)r(ectable)f(job)h(b)n(y)g(getting)g
30191 < (similar)g(v)-5 b(alues)20 b(as)2042 4512 y(SSD)28 b(and)f(exp)r
30192 < (erimen)n(t)h(around)e(290)g(K;)h(ho)n(w)n(ev)n(er,)f(it)i(deviates)
30169 < 2042 4608 y(at)c(b)r(oth)h(higher)f(and)h(lo)n(w)n(er)e(temp)r
30170 < (eratures,)h(failing)h(to)f(predict)2042 4703 y(the)33
30171 < b(exp)r(erimen)n(tal)e(trend.)51 b(TIP5P)31 b(and)i(SSD)g(b)r(oth)f
30172 < (start)g(o\013)2042 4799 y(lo)n(w)i(at)h(the)g(colder)f(temp)r
30173 < (eratures)h(and)g(tend)g(to)g(di\013use)h(to)r(o)2042
30174 < 4894 y(rapidly)c(at)i(the)f(higher)g(temp)r(eratures.)53
30175 < b(This)33 b(t)n(yp)r(e)h(of)f(trend)2042 4990 y(at)e(the)g(higher)f
30176 < (temp)r(eratures)h(is)g(not)g(surprising)e(in)j(that)f(the)2042
30177 < 5085 y(densities)c(of)h(b)r(oth)g(TIP5P)d(and)j(SSD)g(are)e(lo)n(w)n
30178 < (er)g(than)i(exp)r(eri-)2042 5180 y(men)n(tal)d(w)n(ater)g(at)g(temp)r
30179 < (eratures)g(higher)g(than)h(ro)r(om)e(temp)r(er-)2042
30180 < 5276 y(ature.)33 b(When)21 b(calculating)e(the)h(di\013usion)g(co)r
30181 < (e\016cien)n(ts)f(for)g(SSD)2042 5371 y(at)32 b(exp)r(erimen)n(tal)f
30182 < (densities,)i(the)f(resulting)g(v)-5 b(alues)31 b(fall)h(more)p
30191 > (similar)g(v)-5 b(alues)20 b(as)2042 5371 y(SSD)28 b(and)f(exp)r
30192 > (erimen)n(t)h(around)e(290)g(K;)h(ho)n(w)n(ev)n(er,)f(it)i(deviates)p
30193   eop
30194   %%Page: 5 5
30195 < 5 4 bop 4043 -299 a Ft(5)-129 -166 y
30195 > 5 4 bop 4043 -299 a Fu(5)-129 -166 y
30196   gsave currentpoint currentpoint translate -90 neg rotate neg exch
30197   neg exch translate
30198   -129 -166 a @beginspecial
# Line 38165 | Line 38175 | cleartomark countdictstack exch sub { end } repeat res
38175   %%EndDocument
38176   @endspecial 1406 -166 a
38177   currentpoint grestore moveto
38178 < 1406 -166 a -150 1513 a Fq(FIG.)22
38178 > 1406 -166 a -150 1513 a Fr(FIG.)22
38179   b(4:)33 b(Av)n(erage)22 b(di\013usion)f(co)r(e\016cien)n(t)i(o)n(v)n
38180   (er)e(increasing)i(temp)r(era-)-150 1600 y(ture)c(for)i(SSD,)e(SPC/E)
38181 < 543 1568 y Fc(19)609 1600 y Fq(,)i(TIP5P)876 1568 y Fc(4)911
38182 < 1600 y Fq(,)g(and)f(Exp)r(erimen)n(tal)f(data)g(from)-150
38183 < 1687 y(Gillen)27 b Fr(et)h(al.)248 1655 y Fc(21)312 1687
38184 < y Fq(,)e(and)g(from)f(Mills)853 1655 y Fc(22)920 1687
38185 < y Fq(.)-150 1967 y Ft(in)f(line)h(with)f(exp)r(erimen)n(t)g(at)g(these)
38186 < g(temp)r(eratures,)g(alb)r(eit)g(not)-150 2063 y(at)g(standard)e
38187 < (pressure.)35 b(Results)23 b(under)h(these)g(conditions)f(can)-150
38188 < 2158 y(b)r(e)28 b(found)g(later)f(in)h(this)g(pap)r(er.)-15
38189 < 2434 y Fn(C.)88 b(Structural)32 b(Changes)d(and)h(Characterization)-67
38190 < 2648 y Ft(By)e(starting)f(the)h(sim)n(ulations)f(from)g(the)i
38191 < (crystalline)e(state,)-150 2743 y(the)f(melting)h(transition)e(and)h
38192 < (the)g(ice)g(structure)f(can)h(b)r(e)g(stud-)-150 2839
38193 < y(ied)20 b(along)f(with)h(the)h(liquid)f(phase)g(b)r(eha)n(vior)e(b)r
38194 < (ey)n(ond)i(the)g(melt-)-150 2934 y(ing)27 b(p)r(oin)n(t.)37
38181 > 543 1568 y Fc(20)609 1600 y Fr(,)i(TIP5P)876 1568 y Fc(4)911
38182 > 1600 y Fr(,)g(and)f(Exp)r(erimen)n(tal)f(data)g(from)-150
38183 > 1687 y(Gillen)27 b Fs(et)h(al.)248 1655 y Fc(22)312 1687
38184 > y Fr(,)e(and)g(from)f(Mills)853 1655 y Fc(23)920 1687
38185 > y Fr(.)-150 1967 y Fu(at)f(b)r(oth)i(higher)d(and)i(lo)n(w)n(er)e(temp)
38186 > r(eratures,)i(failing)f(to)g(predict)-150 2063 y(the)33
38187 > b(exp)r(erimen)n(tal)f(trend.)51 b(TIP5P)31 b(and)h(SSD)h(b)r(oth)g
38188 > (start)e(o\013)-150 2158 y(lo)n(w)j(at)h(the)h(colder)e(temp)r
38189 > (eratures)g(and)h(tend)g(to)g(di\013use)h(to)r(o)-150
38190 > 2254 y(rapidly)d(at)g(the)g(higher)g(temp)r(eratures.)53
38191 > b(This)34 b(t)n(yp)r(e)f(of)g(trend)-150 2349 y(at)e(the)g(higher)g
38192 > (temp)r(eratures)f(is)h(not)g(surprising)e(in)j(that)f(the)-150
38193 > 2445 y(densities)c(of)h(b)r(oth)g(TIP5P)e(and)h(SSD)h(are)f(lo)n(w)n
38194 > (er)e(than)j(exp)r(eri-)-150 2540 y(men)n(tal)d(w)n(ater)g(at)g(temp)r
38195 > (eratures)g(higher)g(than)h(ro)r(om)e(temp)r(er-)-150
38196 > 2635 y(ature.)34 b(When)20 b(calculating)f(the)h(di\013usion)g(co)r
38197 > (e\016cien)n(ts)f(for)h(SSD)-150 2731 y(at)32 b(exp)r(erimen)n(tal)f
38198 > (densities,)i(the)f(resulting)g(v)-5 b(alues)31 b(fall)h(more)-150
38199 > 2826 y(in)24 b(line)h(with)f(exp)r(erimen)n(t)g(at)g(these)g(temp)r
38200 > (eratures,)g(alb)r(eit)g(not)-150 2922 y(at)g(standard)e(pressure.)35
38201 > b(Results)23 b(under)h(these)g(conditions)f(can)-150
38202 > 3017 y(b)r(e)28 b(found)g(later)f(in)h(this)g(pap)r(er.)-15
38203 > 3294 y Fo(C.)88 b(Structural)32 b(Changes)d(and)h(Characterization)-67
38204 > 3507 y Fu(By)e(starting)f(the)h(sim)n(ulations)f(from)g(the)i
38205 > (crystalline)e(state,)-150 3603 y(the)f(melting)h(transition)e(and)h
38206 > (the)g(ice)g(structure)f(can)h(b)r(e)g(stud-)-150 3698
38207 > y(ied)20 b(along)f(with)h(the)h(liquid)f(phase)g(b)r(eha)n(vior)e(b)r
38208 > (ey)n(ond)i(the)g(melt-)-150 3794 y(ing)27 b(p)r(oin)n(t.)37
38209   b(T)-7 b(o)26 b(lo)r(cate)h(the)g(melting)g(transition,)g(the)g
38210 < (constan)n(t)-150 3030 y(pressure)22 b(heat)i(capacit)n(y)e(\(C)766
38211 < 3042 y Fm(p)807 3030 y Ft(\))i(w)n(as)e(monitored)h(in)h(eac)n(h)f(of)g
38212 < (the)-150 3125 y(sim)n(ulations.)34 b(In)22 b(the)g(melting)f(sim)n
38213 < (ulations)g(of)h(the)g(1024)d(parti-)-150 3221 y(cle)i(ice)g
38214 < Fi(I)122 3233 y Fh(h)187 3221 y Ft(sim)n(ulations,)g(a)g(large)e(spik)n
38215 < (e)i(in)g(C)1252 3233 y Fm(p)1314 3221 y Ft(o)r(ccurs)f(at)h(245)f(K,)
38216 < -150 3316 y(indicating)33 b(a)g(\014rst)g(order)f(phase)g(transition)h
38217 < (for)g(the)g(melting)-150 3412 y(of)h(these)g(ice)f(crystals.)54
38210 > (constan)n(t)-150 3889 y(pressure)22 b(heat)i(capacit)n(y)e(\(C)766
38211 > 3901 y Fn(p)807 3889 y Fu(\))i(w)n(as)e(monitored)h(in)h(eac)n(h)f(of)g
38212 > (the)-150 3984 y(sim)n(ulations.)34 b(In)22 b(the)g(melting)f(sim)n
38213 > (ulations)g(of)h(the)g(1024)d(parti-)-150 4080 y(cle)i(ice)g
38214 > Fj(I)122 4092 y Fi(h)187 4080 y Fu(sim)n(ulations,)g(a)g(large)e(spik)n
38215 > (e)i(in)g(C)1252 4092 y Fn(p)1314 4080 y Fu(o)r(ccurs)f(at)h(245)f(K,)
38216 > -150 4175 y(indicating)33 b(a)g(\014rst)g(order)f(phase)g(transition)h
38217 > (for)g(the)g(melting)-150 4271 y(of)h(these)g(ice)f(crystals.)54
38218   b(When)35 b(the)f(reaction)f(\014eld)h(is)f(turned)-150
38219 < 3507 y(o\013,)22 b(the)g(melting)f(transition)f(o)r(ccurs)g(at)h(235)f
38220 < (K.)h(These)f(melting)-150 3603 y(transitions)25 b(are)h(considerably)e
38221 < (lo)n(w)n(er)h(than)h(the)h(exp)r(erimen)n(tal)-150 3698
38219 > 4366 y(o\013,)22 b(the)g(melting)f(transition)f(o)r(ccurs)g(at)h(235)f
38220 > (K.)h(These)f(melting)-150 4462 y(transitions)25 b(are)h(considerably)e
38221 > (lo)n(w)n(er)h(than)h(the)h(exp)r(erimen)n(tal)-150 4557
38222   y(v)-5 b(alue,)31 b(but)g(this)g(is)f(not)g(surprising)f(in)i(that)g
38223 < (SSD)g(is)f(a)g(simple)-150 3794 y(rigid)d(b)r(o)r(dy)h(mo)r(del)g
38224 < (with)g(a)f(\014xed)g(dip)r(ole.)-67 3889 y(Additional)71
38225 < b(analyses)e(for)i(understanding)f(the)h(melt-)-150 3984
38223 > (SSD)g(is)f(a)g(simple)-150 4653 y(rigid)d(b)r(o)r(dy)h(mo)r(del)g
38224 > (with)g(a)f(\014xed)g(dip)r(ole.)-67 4748 y(Additional)71
38225 > b(analyses)e(for)i(understanding)f(the)h(melt-)-150 4844
38226   y(ing)48 b(phase-transition)e(pro)r(cess)h(w)n(ere)g(p)r(erformed)h
38227 < (via)g(t)n(w)n(o-)-150 4080 y(dimensional)26 b(structure)h(and)f(dip)r
38228 < (ole)h(angle)f(correlations.)34 b(Ex-)-150 4175 y(pressions)26
38229 < b(for)h(the)h(correlations)e(are)g(as)h(follo)n(ws:)-67
38230 < 4474 y Fi(g)-27 4486 y Fm(AB)72 4474 y Ft(\()p Fi(r)n(;)14
38231 < b Ft(cos)g Fi(\022)r Ft(\))23 b(=)172 4593 y Fi(V)p 87
38208 < 4630 238 4 v 87 4706 a(N)154 4718 y Fm(A)207 4706 y Fi(N)274
38209 < 4718 y Fm(B)334 4649 y Fe(h)366 4570 y Ff(X)367 4748
38210 < y Fh(i)p Fs(2)p Fm(A)501 4570 y Ff(X)500 4748 y Fh(j)s
38211 < Fs(2)p Fm(B)636 4649 y Fi(\016)s Ft(\(cos)13 b Fi(\022)21
38212 < b Fe(\000)d Ft(cos)13 b Fi(\022)1140 4661 y Fh(ij)1198
38213 < 4649 y Ft(\))p Fi(\016)s Ft(\()p Fi(r)22 b Fe(\000)c(j)p
38214 < Fg(r)1506 4661 y Fh(ij)1565 4649 y Fe(j)p Ft(\))p Fe(i)28
38215 < b Fi(;)83 b Ft(\(8\))-67 5034 y Fi(g)-27 5046 y Fm(AB)72
38216 < 5034 y Ft(\()p Fi(r)n(;)14 b Ft(cos)g Fi(!)s Ft(\))23
38217 < b(=)146 5153 y Fi(V)p 61 5190 V 61 5266 a(N)128 5278
38218 < y Fm(A)180 5266 y Fi(N)247 5278 y Fm(B)308 5209 y Fe(h)340
38219 < 5130 y Ff(X)341 5308 y Fh(i)p Fs(2)p Fm(A)475 5130 y
38220 < Ff(X)474 5308 y Fh(j)s Fs(2)p Fm(B)610 5209 y Fi(\016)s
38221 < Ft(\(cos)13 b Fi(!)21 b Fe(\000)d Ft(cos)13 b Fi(!)1140
38222 < 5221 y Fh(ij)1198 5209 y Ft(\))p Fi(\016)s Ft(\()p Fi(r)22
38223 < b Fe(\000)c(j)p Fg(r)1506 5221 y Fh(ij)1565 5209 y Fe(j)p
38224 < Ft(\))p Fe(i)28 b Fi(;)83 b Ft(\(9\))2059 1788 y @beginspecial
38225 < 0 @llx 0 @lly 965 @urx 939 @ury 2409 @rwi @setspecial
38227 > (via)g(t)n(w)n(o-)-150 4939 y(dimensional)26 b(structure)h(and)f(dip)r
38228 > (ole)h(angle)f(correlations.)34 b(Ex-)-150 5035 y(pressions)26
38229 > b(for)h(the)h(correlations)e(are)g(as)h(follo)n(ws:)2059
38230 > 1788 y @beginspecial 0 @llx 0 @lly 965 @urx 939 @ury
38231 > 2409 @rwi @setspecial
38232   %%BeginDocument: fullContours.eps
38233   %!PS-Adobe-3.1 EPSF-3.0
38234   %%Title: fullContours.eps
# Line 73310 | Line 73316 | userdict /ai9_skip_data get exec
73316   %AI9_PrivateDataEnd
73317  
73318   %%EndDocument
73319 < @endspecial 2042 1958 a Fq(FIG.)27 b(5:)39 b(Con)n(tour)27
73320 < b(plots)h(of)g(2D)g(angular)g(g\()p Fp(r)r Fq(\)'s)g(for)g(512)g(SSD)e
73319 > @endspecial 2042 1958 a Fr(FIG.)g(5:)39 b(Con)n(tour)27
73320 > b(plots)h(of)g(2D)g(angular)g(g\()p Fq(r)r Fr(\)'s)g(for)g(512)g(SSD)e
73321   (sys-)2042 2045 y(tems)h(at)h(100)h(K)e(\(A)g(&)h(B\))g(and)f(300)i(K)e
73322   (\(C)h(&)g(D\).)f(Con)n(tour)i(colors)2042 2132 y(are)i(in)n(v)n(erted)
73323   e(for)i(clarit)n(y:)45 b(dark)30 b(areas)h(signify)h(p)r(eaks)e(while)i
73324   (ligh)n(t)2042 2219 y(areas)24 b(signify)f(depressions.)35
73325 < b(White)22 b(areas)i(ha)n(v)n(e)e(g\()p Fr(r)8 b Fq(\))23
73325 > b(White)22 b(areas)i(ha)n(v)n(e)e(g\()p Fs(r)8 b Fr(\))23
73326   b(v)l(alues)g(b)r(elo)n(w)2042 2307 y(0.5)k(and)e(blac)n(k)g(areas)i
73327   (ha)n(v)n(e)e(v)l(alues)h(ab)r(o)n(v)n(e)g(1.5.)2531
73328   3258 y @beginspecial 0 @llx 0 @lly 182 @urx 143 @ury
# Line 79451 | Line 79457 | b(dimensional)f(illustration)i(of)f(the)f(angles)h(in)
79457   @endspecial 2042 3428 a(FIG.)31 b(6:)46 b(Tw)n(o)32
79458   b(dimensional)f(illustration)i(of)f(the)f(angles)h(in)n(v)n(olv)n(ed)
79459   2042 3515 y(in)25 b(the)h(correlations)h(observ)n(ed)f(in)f(\014gure)h
79460 < (5.)2042 3796 y Ft(where)19 b Fi(\022)i Ft(and)f Fi(!)i
79461 < Ft(refer)c(to)h(the)h(angles)e(sho)n(wn)h(in)h(the)f(ab)r(o)n(v)n(e)f
79462 < (illus-)2042 3891 y(tration.)36 b(By)26 b(binning)g(o)n(v)n(er)f(b)r
79463 < (oth)i(distance)f(and)g(the)h(cosine)e(of)2042 3987 y(the)31
79464 < b(desired)g(angle)f(b)r(et)n(w)n(een)h(the)h(t)n(w)n(o)e(dip)r(oles,)i
79465 < (the)f(g\()p Fl(r)9 b Ft(\))32 b(can)2042 4082 y(b)r(e)37
79466 < b(dissected)g(to)g(determine)g(the)h(common)f(dip)r(ole)g(arrange-)2042
79467 < 4178 y(men)n(ts)29 b(that)g(constitute)g(the)h(p)r(eaks)e(and)h
79468 < (troughs.)40 b(F)-7 b(rames)28 b(A)2042 4273 y(and)d(B)h(of)f(\014gure)
79469 < g(5)g(sho)n(w)g(a)g(relativ)n(ely)f(crystalline)h(state)g(of)g(an)2042
79470 < 4368 y(ice)36 b Fi(I)2211 4380 y Fh(c)2281 4368 y Ft(sim)n(ulation.)62
79471 < b(The)36 b(\014rst)g(p)r(eak)g(of)g(the)g(g\()p Fl(r)9
79472 < b Ft(\))36 b(primarily)2042 4464 y(consists)23 b(of)h(the)g(preferred)f
79473 < (h)n(ydrogen)f(b)r(onding)i(arrangemen)n(ts)2042 4559
79474 < y(as)i(dictated)h(b)n(y)g(the)h(tetrahedral)d(stic)n(ky)i(p)r(oten)n
79475 < (tial,)g(one)f(p)r(eak)2042 4655 y(for)k(the)i(donating)e(and)h(the)g
79476 < (other)f(for)h(the)g(accepting)g(h)n(ydro-)2042 4750
79477 < y(gen)39 b(b)r(onds.)73 b(Due)40 b(to)g(the)g(high)f(degree)g(of)h
79478 < (crystallinit)n(y)e(of)2042 4846 y(the)e(sample,)i(the)f(second)e(and)h
79479 < (third)g(solv)-5 b(ation)35 b(shells)h(sho)n(w)2042 4941
79480 < y(a)30 b(rep)r(eated)h(p)r(eak)f(arrangemen)n(t)f(whic)n(h)h(deca)n(ys)
79481 < g(at)h(distances)2042 5037 y(around)19 b(the)j(fourth)e(solv)-5
79482 < b(ation)20 b(shell,)i(near)e(the)h(imp)r(osed)g(cuto\013)2042
79483 < 5132 y(for)27 b(the)h(Lennard-Jones)e(and)i(dip)r(ole-dip)r(ole)g(in)n
79484 < (teractions.)36 b(In)2042 5228 y(the)19 b(higher)g(temp)r(erature)f
79485 < (sim)n(ulation)h(sho)n(wn)f(in)i(frames)e(C)h(and)2042
79486 < 5323 y(D,)35 b(the)g(rep)r(eated)f(p)r(eak)g(features)g(are)g
79487 < (signi\014can)n(tly)g(blurred.)p eop
79460 > (5.)2125 3999 y Fj(g)2165 4011 y Fn(AB)2264 3999 y Fu(\()p
79461 > Fj(r)n(;)14 b Fu(cos)f Fj(\022)r Fu(\))24 b(=)2364 4118
79462 > y Fj(V)p 2278 4155 238 4 v 2278 4231 a(N)2345 4243 y
79463 > Fn(A)2398 4231 y Fj(N)2465 4243 y Fn(B)2526 4174 y Ff(h)2558
79464 > 4095 y Fg(X)2559 4273 y Fi(i)p Ft(2)p Fn(A)2693 4095
79465 > y Fg(X)2692 4273 y Fi(j)s Ft(2)p Fn(B)2827 4174 y Fj(\016)s
79466 > Fu(\(cos)14 b Fj(\022)20 b Ff(\000)f Fu(cos)13 b Fj(\022)3332
79467 > 4186 y Fi(ij)3390 4174 y Fu(\))p Fj(\016)s Fu(\()p Fj(r)22
79468 > b Ff(\000)c(j)p Fh(r)3698 4186 y Fi(ij)3757 4174 y Ff(j)p
79469 > Fu(\))p Ff(i)28 b Fj(;)83 b Fu(\(8\))2125 4559 y Fj(g)2165
79470 > 4571 y Fn(AB)2264 4559 y Fu(\()p Fj(r)n(;)14 b Fu(cos)f
79471 > Fj(!)s Fu(\))23 b(=)2338 4677 y Fj(V)p 2252 4714 V 2252
79472 > 4790 a(N)2319 4802 y Fn(A)2372 4790 y Fj(N)2439 4802
79473 > y Fn(B)2499 4733 y Ff(h)2531 4655 y Fg(X)2532 4833 y
79474 > Fi(i)p Ft(2)p Fn(A)2667 4655 y Fg(X)2666 4833 y Fi(j)s
79475 > Ft(2)p Fn(B)2801 4733 y Fj(\016)s Fu(\(cos)14 b Fj(!)21
79476 > b Ff(\000)d Fu(cos)13 b Fj(!)3332 4745 y Fi(ij)3390 4733
79477 > y Fu(\))p Fj(\016)s Fu(\()p Fj(r)22 b Ff(\000)c(j)p Fh(r)3698
79478 > 4745 y Fi(ij)3757 4733 y Ff(j)p Fu(\))p Ff(i)28 b Fj(;)83
79479 > b Fu(\(9\))2042 5001 y(where)19 b Fj(\022)i Fu(and)f
79480 > Fj(!)i Fu(refer)c(to)h(the)h(angles)e(sho)n(wn)h(in)h(the)f(ab)r(o)n(v)
79481 > n(e)f(illus-)2042 5097 y(tration.)36 b(By)26 b(binning)g(o)n(v)n(er)f
79482 > (b)r(oth)i(distance)f(and)g(the)h(cosine)e(of)2042 5192
79483 > 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
79484 > (oles,)i(the)f(g\()p Fm(r)9 b Fu(\))32 b(can)2042 5288
79485 > y(b)r(e)37 b(dissected)g(to)g(determine)g(the)h(common)f(dip)r(ole)g
79486 > (arrange-)2042 5383 y(men)n(ts)29 b(that)g(constitute)g(the)h(p)r(eaks)
79487 > e(and)h(troughs.)40 b(F)-7 b(rames)28 b(A)2042 5479 y(and)d(B)h(of)f
79488 > (\014gure)g(5)g(sho)n(w)g(a)g(relativ)n(ely)f(crystalline)h(state)g(of)
79489 > g(an)p eop
79490   %%Page: 6 6
79491 < 6 5 bop 4043 -299 a Ft(6)-150 -83 y(The)21 b(\014rst)g(solv)-5
79491 > 6 5 bop 4043 -299 a Fu(6)-150 -83 y(ice)36 b Fj(I)19
79492 > -71 y Fi(c)89 -83 y Fu(sim)n(ulation.)62 b(The)36 b(\014rst)g(p)r(eak)g
79493 > (of)g(the)g(g\()p Fm(r)9 b Fu(\))36 b(primarily)-150
79494 > 12 y(consists)23 b(of)h(the)g(preferred)f(h)n(ydrogen)f(b)r(onding)i
79495 > (arrangemen)n(ts)-150 108 y(as)i(dictated)i(b)n(y)e(the)i(tetrahedral)e
79496 > (stic)n(ky)g(p)r(oten)n(tial,)h(one)g(p)r(eak)-150 203
79497 > y(for)j(the)i(donating)e(and)h(the)g(other)g(for)f(the)i(accepting)e(h)
79498 > n(ydro-)-150 299 y(gen)39 b(b)r(onds.)73 b(Due)40 b(to)g(the)g(high)g
79499 > (degree)e(of)i(crystallinit)n(y)e(of)-150 394 y(the)e(sample,)i(the)f
79500 > (second)e(and)h(third)g(solv)-5 b(ation)36 b(shells)f(sho)n(w)-150
79501 > 490 y(a)30 b(rep)r(eated)h(p)r(eak)f(arrangemen)n(t)f(whic)n(h)i(deca)n
79502 > (ys)e(at)i(distances)-150 585 y(around)20 b(the)h(fourth)g(solv)-5
79503 > b(ation)19 b(shell,)j(near)e(the)h(imp)r(osed)g(cuto\013)-150
79504 > 681 y(for)27 b(the)i(Lennard-Jones)c(and)j(dip)r(ole-dip)r(ole)g(in)n
79505 > (teractions.)36 b(In)-150 776 y(the)20 b(higher)e(temp)r(erature)h(sim)
79506 > n(ulation)f(sho)n(wn)h(in)g(frames)f(C)i(and)-150 872
79507 > y(D,)35 b(the)g(rep)r(eated)f(p)r(eak)h(features)f(are)f(signi\014can)n
79508 > (tly)h(blurred.)-150 967 y(The)21 b(\014rst)g(solv)-5
79509   b(ation)20 b(shell)h(still)h(sho)n(ws)e(the)h(strong)f(e\013ect)i(of)f
79510 < (the)-150 12 y(stic)n(ky-p)r(oten)n(tial,)j(although)f(it)i(co)n(v)n
79511 < (ers)c(a)j(larger)e(area,)i(extend-)-150 108 y(ing)33
79510 > (the)-150 1063 y(stic)n(ky-p)r(oten)n(tial,)j(although)f(it)i(co)n(v)n
79511 > (ers)c(a)j(larger)e(area,)i(extend-)-150 1158 y(ing)33
79512   b(to)g(include)h(a)f(fraction)g(of)g(aligned)f(dip)r(ole)i(p)r(eaks)f
79513 < (within)-150 203 y(the)e(\014rst)f(solv)-5 b(ation)29
79513 > (within)-150 1254 y(the)e(\014rst)f(solv)-5 b(ation)29
79514   b(shell.)45 b(The)30 b(latter)g(p)r(eaks)g(lose)f(de\014nition)-150
79515 < 299 y(as)g(thermal)g(motion)h(and)f(the)h(comp)r(eting)g(dip)r(ole)g
79516 < (force)f(o)n(v)n(er-)-150 394 y(comes)23 b(the)i(stic)n(ky)e(p)r(oten)n
79517 < (tial's)g(tigh)n(t)h(tetrahedral)f(structuring)-150 490
79518 < y(of)28 b(the)g(\015uid.)-67 585 y(This)k(complex)g(in)n(terpla)n(y)f
79519 < (b)r(et)n(w)n(een)h(dip)r(ole)h(and)f(stic)n(ky)f(in-)-150
79520 < 681 y(teractions)37 b(w)n(as)g(remark)n(ed)f(up)r(on)i(as)f(a)h(p)r
79521 < (ossible)g(reason)e(for)-150 776 y(the)25 b(split)f(second)g(p)r(eak)g
79522 < (in)g(the)h(o)n(xygen-o)n(xygen)c(g\()p Fl(r)9 b Ft(\).)1592
79523 < 746 y Fm(5)1654 776 y Ft(A)n(t)24 b(lo)n(w)-150 872 y(temp)r(eratures,)
79524 < h(the)h(second)f(solv)-5 b(ation)24 b(shell)h(p)r(eak)g(app)r(ears)g
79525 < (to)-150 967 y(ha)n(v)n(e)k(t)n(w)n(o)h(distinct)h(parts)f(that)g
79526 < (blend)h(together)e(to)i(form)f(one)-150 1063 y(observ)-5
79527 < b(able)22 b(p)r(eak.)36 b(A)n(t)23 b(higher)g(temp)r(eratures,)h(this)g
79528 < (split)g(c)n(har-)-150 1158 y(acter)k(alters)h(to)g(sho)n(w)f(the)i
79529 < (leading)e(4)1101 1143 y(\027)1101 1158 y(A)i(p)r(eak)f(dominated)g(b)n
79530 < (y)-150 1254 y(equatorial)i(an)n(ti-parallel)h(dip)r(ole)h(orien)n
79531 < (tations,)g(and)g(there)g(is)-150 1349 y(tigh)n(tly)k(bunc)n(hed)h
79532 < (group)f(of)g(axially)f(arranged)g(dip)r(oles)h(that)-150
79533 < 1445 y(most)29 b(lik)n(ely)f(consist)h(of)f(the)i(smaller)e(fraction)g
79534 < (aligned)g(dip)r(ole)-150 1540 y(pairs.)36 b(The)27 b(trailing)f(part)g
79535 < (of)h(the)g(split)h(p)r(eak)e(at)h(5)1513 1525 y(\027)1513
79536 < 1540 y(A)g(is)g(domi-)-150 1636 y(nated)f(b)n(y)g(aligned)g(dip)r(oles)
79537 < g(that)g(range)f(primarily)g(within)i(the)-150 1731 y(axial)c(to)h(the)
79538 < h(c)n(hief)f(h)n(ydrogen)e(b)r(ond)j(arrangemen)n(ts)c(similar)j(to)
79539 < -150 1826 y(those)g(seen)g(in)h(the)f(\014rst)h(solv)-5
79540 < b(ation)23 b(shell.)36 b(This)24 b(evidence)g(indi-)-150
79541 < 1922 y(cates)h(that)g(the)h(dip)r(ole)f(pair)g(in)n(teraction)f(b)r
79542 < (egins)h(to)h(dominate)-150 2017 y(outside)31 b(of)g(the)g(range)f(of)h
79543 < (the)g(dip)r(olar)g(repulsion)f(term,)i(with)-150 2113
79515 > 1349 y(as)g(thermal)g(motion)h(and)f(the)h(comp)r(eting)g(dip)r(ole)g
79516 > (force)f(o)n(v)n(er-)-150 1445 y(comes)23 b(the)i(stic)n(ky)e(p)r(oten)
79517 > n(tial's)g(tigh)n(t)h(tetrahedral)f(structuring)-150
79518 > 1540 y(of)28 b(the)g(\015uid.)-67 1636 y(This)k(complex)g(in)n(terpla)n
79519 > (y)f(b)r(et)n(w)n(een)h(dip)r(ole)h(and)f(stic)n(ky)f(in-)-150
79520 > 1731 y(teractions)37 b(w)n(as)g(remark)n(ed)f(up)r(on)i(as)f(a)h(p)r
79521 > (ossible)g(reason)e(for)-150 1826 y(the)25 b(split)f(second)g(p)r(eak)g
79522 > (in)g(the)h(o)n(xygen-o)n(xygen)c(g\()p Fm(r)9 b Fu(\).)1592
79523 > 1796 y Fn(5)1654 1826 y Fu(A)n(t)24 b(lo)n(w)-150 1922
79524 > y(temp)r(eratures,)h(the)h(second)f(solv)-5 b(ation)24
79525 > 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)
79526 > h(distinct)h(parts)f(that)g(blend)h(together)e(to)i(form)f(one)-150
79527 > 2113 y(observ)-5 b(able)22 b(p)r(eak.)36 b(A)n(t)23 b(higher)g(temp)r
79528 > (eratures,)h(this)g(split)g(c)n(har-)-150 2208 y(acter)k(alters)h(to)g
79529 > (sho)n(w)f(the)i(leading)e(4)1101 2193 y(\027)1101 2208
79530 > y(A)i(p)r(eak)f(dominated)g(b)n(y)-150 2304 y(equatorial)i(an)n
79531 > (ti-parallel)h(dip)r(ole)h(orien)n(tations,)g(and)g(there)g(is)-150
79532 > 2399 y(tigh)n(tly)k(bunc)n(hed)h(group)f(of)g(axially)f(arranged)g(dip)
79533 > r(oles)h(that)-150 2495 y(most)29 b(lik)n(ely)f(consist)h(of)f(the)i
79534 > (smaller)e(fraction)g(aligned)g(dip)r(ole)-150 2590 y(pairs.)36
79535 > b(The)27 b(trailing)f(part)g(of)h(the)g(split)h(p)r(eak)e(at)h(5)1513
79536 > 2575 y(\027)1513 2590 y(A)g(is)g(domi-)-150 2686 y(nated)f(b)n(y)g
79537 > (aligned)g(dip)r(oles)g(that)g(range)f(primarily)g(within)i(the)-150
79538 > 2781 y(axial)c(to)h(the)h(c)n(hief)f(h)n(ydrogen)e(b)r(ond)j
79539 > (arrangemen)n(ts)c(similar)j(to)-150 2877 y(those)g(seen)g(in)h(the)f
79540 > (\014rst)h(solv)-5 b(ation)23 b(shell.)36 b(This)24 b(evidence)g(indi-)
79541 > -150 2972 y(cates)h(that)g(the)h(dip)r(ole)f(pair)g(in)n(teraction)f(b)
79542 > r(egins)h(to)h(dominate)-150 3068 y(outside)31 b(of)g(the)g(range)f(of)
79543 > h(the)g(dip)r(olar)g(repulsion)f(term,)i(with)-150 3163
79544   y(the)e(primary)f(energetically)f(fa)n(v)n(orable)g(dip)r(ole)i
79545 < (arrangemen)n(ts)-150 2208 y(p)r(opulating)j(the)h(region)e
79546 < (immediately)i(outside)g(of)f(it's)h(range)-150 2304
79547 < y(\(around)24 b(4)228 2289 y(\027)228 2304 y(A\),)i(and)f(arrangemen)n
79548 < (ts)e(that)j(seek)e(to)h(ideally)g(sat-)-150 2399 y(isfy)33
79545 > (arrangemen)n(ts)-150 3259 y(p)r(opulating)j(the)h(region)e
79546 > (immediately)i(outside)g(of)f(it's)h(range)-150 3354
79547 > y(\(around)24 b(4)228 3339 y(\027)228 3354 y(A\),)i(and)f(arrangemen)n
79548 > (ts)e(that)j(seek)e(to)h(ideally)g(sat-)-150 3450 y(isfy)33
79549   b(b)r(oth)g(the)g(stic)n(ky)f(and)g(dip)r(ole)h(forces)f(lo)r(cate)g
79550 < (themselv)n(es)-150 2495 y(just)c(b)r(ey)n(ond)f(this)h(region)f
79551 < (\(around)g(5)1097 2480 y(\027)1097 2495 y(A\).)-67 2590
79550 > (themselv)n(es)-150 3545 y(just)c(b)r(ey)n(ond)f(this)h(region)f
79551 > (\(around)g(5)1097 3530 y(\027)1097 3545 y(A\).)-67 3641
79552   y(F)-7 b(rom)25 b(these)h(\014ndings,)f(the)h(split)g(second)f(p)r(eak)
79553 < g(is)g(primarily)-150 2686 y(the)35 b(pro)r(duct)g(of)f(the)i(dip)r
79553 > g(is)g(primarily)-150 3736 y(the)35 b(pro)r(duct)g(of)f(the)i(dip)r
79554   (olar)e(repulsion)g(term)g(of)h(the)g(stic)n(ky)-150
79555 < 2781 y(p)r(oten)n(tial.)56 b(In)34 b(fact,)h(the)g(leading)e(of)h(the)g
79556 < (t)n(w)n(o)f(p)r(eaks)h(can)f(b)r(e)-150 2877 y(pushed)25
79555 > 3831 y(p)r(oten)n(tial.)56 b(In)34 b(fact,)h(the)g(leading)e(of)h(the)g
79556 > (t)n(w)n(o)f(p)r(eaks)h(can)f(b)r(e)-150 3927 y(pushed)25
79557   b(out)h(and)f(merged)f(with)i(the)g(outer)e(split)i(p)r(eak)f(just)h(b)
79558 < n(y)-150 2972 y(extending)h(the)g(switc)n(hing)f(function)i(cuto\013)f
79559 < (\()p Fi(s)1366 2942 y Fs(0)1389 2972 y Ft(\()p Fi(r)1458
79560 < 2984 y Fh(ij)1517 2972 y Ft(\)\))h(from)e(its)-150 3077
79561 < y(normal)k(4.0)272 3062 y(\027)272 3077 y(A)h(to)g(v)-5
79562 < b(alues)31 b(of)g(4.5)f(or)g(ev)n(en)g(5)1326 3062 y(\027)1326
79563 < 3077 y(A.)h(This)g(t)n(yp)r(e)g(of)-150 3172 y(correction)f(is)i(not)g
79558 > n(y)-150 4022 y(extending)h(the)g(switc)n(hing)f(function)i(cuto\013)f
79559 > (\()p Fj(s)1366 3992 y Ft(0)1389 4022 y Fu(\()p Fj(r)1458
79560 > 4034 y Fi(ij)1517 4022 y Fu(\)\))h(from)e(its)-150 4127
79561 > y(normal)k(4.0)272 4112 y(\027)272 4127 y(A)h(to)g(v)-5
79562 > b(alues)31 b(of)g(4.5)f(or)g(ev)n(en)g(5)1326 4112 y(\027)1326
79563 > 4127 y(A.)h(This)g(t)n(yp)r(e)g(of)-150 4222 y(correction)f(is)i(not)g
79564   (recommended)f(for)g(impro)n(ving)g(the)h(liquid)-150
79565 < 3268 y(structure,)c(b)r(ecause)f(the)h(second)g(solv)-5
79566 < b(ation)27 b(shell)h(will)g(still)g(b)r(e)-150 3363 y(shifted)g(to)r(o)
79565 > 4318 y(structure,)c(b)r(ecause)f(the)h(second)g(solv)-5
79566 > b(ation)27 b(shell)h(will)g(still)g(b)r(e)-150 4413 y(shifted)g(to)r(o)
79567   e(far)g(out.)37 b(In)27 b(addition,)g(this)g(w)n(ould)g(ha)n(v)n(e)e
79568 < (an)i(ev)n(en)-150 3458 y(more)i(detrimen)n(tal)h(e\013ect)g(on)g(the)h
79569 < (system)e(densities,)i(leading)-150 3554 y(to)40 b(a)g(liquid)h(with)f
79568 > (an)i(ev)n(en)-150 4509 y(more)i(detrimen)n(tal)h(e\013ect)g(on)g(the)h
79569 > (system)e(densities,)i(leading)-150 4604 y(to)40 b(a)g(liquid)h(with)f
79570   (a)g(more)g(op)r(en)g(structure)g(and)g(a)g(densit)n(y)-150
79571 < 3649 y(considerably)24 b(lo)n(w)n(er)f(than)i(the)h(normal)e(SSD)h(b)r
79572 < (eha)n(vior)f(sho)n(wn)-150 3745 y(previously)-7 b(.)47
79571 > 4700 y(considerably)24 b(lo)n(w)n(er)f(than)i(the)h(normal)e(SSD)h(b)r
79572 > (eha)n(vior)f(sho)n(wn)-150 4795 y(previously)-7 b(.)47
79573   b(A)31 b(b)r(etter)h(correction)e(w)n(ould)h(b)r(e)g(to)g(include)h
79574 < (the)-150 3840 y(quadrup)r(ole-quadrup)r(ole)e(in)n(teractions)h(for)h
79575 < (the)g(w)n(ater)f(parti-)-150 3936 y(cles)h(outside)h(of)f(the)h
79574 > (the)-150 4891 y(quadrup)r(ole-quadrup)r(ole)e(in)n(teractions)h(for)h
79575 > (the)g(w)n(ater)f(parti-)-150 4986 y(cles)h(outside)h(of)f(the)h
79576   (\014rst)g(solv)-5 b(ation)31 b(shell,)j(but)f(this)g(reduces)-150
79577 < 4031 y(the)g(simplicit)n(y)f(and)h(sp)r(eed)g(adv)-5
79577 > 5082 y(the)g(simplicit)n(y)f(and)h(sp)r(eed)g(adv)-5
79578   b(an)n(tage)30 b(of)j(SSD,)g(so)f(it)h(is)f(not)-150
79579 < 4127 y(the)c(most)f(desirable)g(path)h(to)f(tak)n(e.)-34
79580 < 4403 y Fn(D.)88 b(Adjusted)29 b(P)n(oten)n(tials:)40
79581 < b(SSD/E)30 b(and)f(SSD/RF)-67 4617 y Ft(The)j(prop)r(ensit)n(y)g(of)g
79582 < (SSD)h(to)f(adopt)f(lo)n(w)n(er)g(than)h(exp)r(ected)-150
79583 < 4712 y(densities)21 b(under)h(v)-5 b(arying)20 b(conditions)h(is)g
79584 < (troubling,)h(esp)r(ecially)-150 4807 y(at)32 b(higher)f(temp)r
79585 < (eratures.)50 b(In)32 b(order)f(to)h(correct)f(this)h(b)r(eha)n(v-)-150
79586 < 4903 y(ior,)25 b(it's)h(necessary)e(to)h(adjust)h(the)g(force)e
79587 < (\014eld)i(parameters)e(for)-150 4998 y(the)g(primary)e(in)n
79588 < (termolecular)g(in)n(teractions.)35 b(In)24 b(undergoing)e(a)-150
79589 < 5094 y(reparameterization,)31 b(it)h(is)g(imp)r(ortan)n(t)f(not)h(to)g
79590 < (fo)r(cus)g(on)g(just)-150 5189 y(one)23 b(prop)r(ert)n(y)f(and)h
79591 < (neglect)g(the)h(other)e(imp)r(ortan)n(t)h(prop)r(erties.)-150
79592 < 5285 y(In)38 b(this)h(case,)h(it)f(w)n(ould)f(b)r(e)h(ideal)f(to)g
79593 < (correct)f(the)h(densities)-150 5380 y(while)28 b(main)n(taining)f(the)
79594 < h(accurate)e(transp)r(ort)h(prop)r(erties.)2070 -31 y
79595 < Fq(T)-6 b(ABLE)26 b(I:)g(P)n(arameters)g(for)g(the)f(original)j(and)d
79596 < (adjusted)h(mo)r(dels)p 2228 12 1644 4 v 2270 94 a(P)n(arameters)260
79597 < b(SSD)3054 63 y Fk(y)3222 94 y Fq(SSD/E)84 b(SSD/RF)p
79598 < 2228 124 V 2322 205 a Fp(\033)28 b Fq(\()2424 192 y(\027)2424
79599 < 205 y(A\))398 b(3.051)169 b(3.035)k(3.019)2322 292 y
79600 < Fp(\017)25 b Fq(\(k)n(cal/mol\))178 b(0.152)169 b(0.152)k(0.152)2322
79601 < 379 y Fp(\026)26 b Fq(\(D\))417 b(2.35)187 b(2.418)173
79602 < b(2.480)2322 467 y Fp(\027)2360 475 y Fc(0)2420 467 y
79603 < Fq(\(k)n(cal/mol\))117 b(3.7284)169 b(3.90)211 b(3.90)2322
79604 < 558 y Fp(r)2357 567 y Fo(l)2406 558 y Fq(\()2436 545
79605 < y(\027)2436 558 y(A\))406 b(2.75)206 b(2.40)211 b(2.40)2322
79606 < 649 y Fp(r)2357 657 y Fo(u)2423 649 y Fq(\()2453 636
79607 < y(\027)2453 649 y(A\))389 b(3.35)206 b(3.80)211 b(3.80)2322
79608 < 736 y Fp(\027)2365 705 y Fk(0)2360 749 y Fc(0)2420 736
79609 < y Fq(\(k)n(cal/mol\))117 b(3.7284)169 b(3.90)211 b(3.90)2322
79610 < 828 y Fp(r)2359 796 y Fk(0)2357 843 y Fo(l)2406 828 y
79611 < Fq(\()2436 815 y(\027)2436 828 y(A\))406 b(2.75)206 b(2.75)211
79612 < b(2.75)2322 919 y Fp(r)2359 887 y Fk(0)2357 932 y Fo(u)2423
79613 < 919 y Fq(\()2453 906 y(\027)2453 919 y(A\))389 b(4.00)206
79614 < b(3.35)211 b(3.35)2245 1020 y Fk(y)2303 1051 y Fq(ref.)35
79615 < b(5)2125 1326 y Ft(The)22 b(p)r(ossible)h(parameters)d(for)i(tuning)h
79616 < (include)g(the)g Fi(\033)j Ft(and)c Fi(\017)2042 1422
79617 < y Ft(Lennard-Jones)28 b(parameters,)h(the)h(dip)r(ole)g(strength)g(\()p
79618 < Fi(\026)p Ft(\),)h(and)2042 1517 y(the)20 b(stic)n(ky)f(attractiv)n(e)g
79619 < (and)g(dip)r(ole)h(repulsiv)n(e)f(terms)g(with)h(their)2042
79620 < 1613 y(resp)r(ectiv)n(e)31 b(cuto\013s.)51 b(T)-7 b(o)31
79621 < b(alter)h(the)g(attractiv)n(e)f(and)h(repulsiv)n(e)2042
79622 < 1708 y(terms)h(of)g(the)h(stic)n(ky)f(p)r(oten)n(tial)g(indep)r(enden)n
79623 < (tly)-7 b(,)36 b(it)e(is)f(neces-)2042 1804 y(sary)26
79579 > 5177 y(the)c(most)f(desirable)g(path)h(to)f(tak)n(e.)2070
79580 > -31 y Fr(T)-6 b(ABLE)26 b(I:)g(P)n(arameters)g(for)g(the)f(original)j
79581 > (and)d(adjusted)h(mo)r(dels)p 2228 12 1644 4 v 2270 94
79582 > a(P)n(arameters)260 b(SSD)3054 63 y Fl(y)3222 94 y Fr(SSD/E)84
79583 > b(SSD/RF)p 2228 124 V 2322 205 a Fq(\033)28 b Fr(\()2424
79584 > 192 y(\027)2424 205 y(A\))398 b(3.051)169 b(3.035)k(3.019)2322
79585 > 292 y Fq(\017)25 b Fr(\(k)n(cal/mol\))178 b(0.152)169
79586 > b(0.152)k(0.152)2322 379 y Fq(\026)26 b Fr(\(D\))417
79587 > b(2.35)187 b(2.418)173 b(2.480)2322 467 y Fq(\027)2360
79588 > 475 y Fc(0)2420 467 y Fr(\(k)n(cal/mol\))117 b(3.7284)169
79589 > b(3.90)211 b(3.90)2322 558 y Fq(r)2357 567 y Fp(l)2406
79590 > 558 y Fr(\()2436 545 y(\027)2436 558 y(A\))406 b(2.75)206
79591 > b(2.40)211 b(2.40)2322 649 y Fq(r)2357 657 y Fp(u)2423
79592 > 649 y Fr(\()2453 636 y(\027)2453 649 y(A\))389 b(3.35)206
79593 > b(3.80)211 b(3.80)2322 736 y Fq(\027)2365 705 y Fl(0)2360
79594 > 749 y Fc(0)2420 736 y Fr(\(k)n(cal/mol\))117 b(3.7284)169
79595 > b(3.90)211 b(3.90)2322 828 y Fq(r)2359 796 y Fl(0)2357
79596 > 843 y Fp(l)2406 828 y Fr(\()2436 815 y(\027)2436 828
79597 > y(A\))406 b(2.75)206 b(2.75)211 b(2.75)2322 919 y Fq(r)2359
79598 > 887 y Fl(0)2357 932 y Fp(u)2423 919 y Fr(\()2453 906
79599 > y(\027)2453 919 y(A\))389 b(4.00)206 b(3.35)211 b(3.35)2245
79600 > 1020 y Fl(y)2303 1051 y Fr(ref.)35 b(5)2158 1326 y Fo(D.)87
79601 > b(Adjusted)30 b(P)n(oten)n(tials:)40 b(SSD/E)29 b(and)h(SSD/RF)2125
79602 > 1540 y Fu(The)i(prop)r(ensit)n(y)f(of)h(SSD)h(to)f(adopt)g(lo)n(w)n(er)
79603 > f(than)h(exp)r(ected)2042 1636 y(densities)21 b(under)g(v)-5
79604 > b(arying)21 b(conditions)f(is)i(troubling,)g(esp)r(ecially)2042
79605 > 1731 y(at)32 b(higher)f(temp)r(eratures.)50 b(In)32 b(order)f(to)h
79606 > (correct)f(this)h(b)r(eha)n(v-)2042 1826 y(ior,)25 b(it's)h(necessary)d
79607 > (to)j(adjust)g(the)f(force)g(\014eld)h(parameters)e(for)2042
79608 > 1922 y(the)g(primary)e(in)n(termolecular)g(in)n(teractions.)35
79609 > b(In)23 b(undergoing)g(a)2042 2017 y(reparameterization,)30
79610 > b(it)j(is)f(imp)r(ortan)n(t)f(not)h(to)g(fo)r(cus)g(on)g(just)2042
79611 > 2113 y(one)23 b(prop)r(ert)n(y)f(and)h(neglect)g(the)g(other)g(imp)r
79612 > (ortan)n(t)g(prop)r(erties.)2042 2208 y(In)38 b(this)h(case,)h(it)f(w)n
79613 > (ould)f(b)r(e)g(ideal)g(to)h(correct)d(the)j(densities)2042
79614 > 2304 y(while)28 b(main)n(taining)e(the)i(accurate)f(transp)r(ort)f
79615 > (prop)r(erties.)2125 2399 y(The)c(p)r(ossible)h(parameters)d(for)i
79616 > (tuning)h(include)g(the)g Fj(\033)j Fu(and)c Fj(\017)2042
79617 > 2495 y Fu(Lennard-Jones)28 b(parameters,)h(the)h(dip)r(ole)g(strength)g
79618 > (\()p Fj(\026)p Fu(\),)h(and)2042 2590 y(the)20 b(stic)n(ky)f
79619 > (attractiv)n(e)g(and)g(dip)r(ole)h(repulsiv)n(e)f(terms)g(with)h(their)
79620 > 2042 2686 y(resp)r(ectiv)n(e)31 b(cuto\013s.)51 b(T)-7
79621 > b(o)31 b(alter)h(the)g(attractiv)n(e)f(and)h(repulsiv)n(e)2042
79622 > 2781 y(terms)h(of)g(the)h(stic)n(ky)f(p)r(oten)n(tial)g(indep)r(enden)n
79623 > (tly)-7 b(,)36 b(it)e(is)f(neces-)2042 2877 y(sary)26
79624   b(to)i(separate)e(the)i(terms)f(as)g(follo)n(ws:)2150
79625 < 2003 y Fi(u)2198 1963 y Fh(sp)2198 2026 y(ij)2267 2003
79626 < y Ft(\()p Fg(r)2338 2015 y Fh(ij)2398 2003 y Fi(;)14
79627 < b Fg(\012)2503 2015 y Fh(i)2531 2003 y Fi(;)g Fg(\012)2637
79628 < 2015 y Fh(j)2672 2003 y Ft(\))23 b(=)2825 1947 y Fi(\027)2866
79629 < 1959 y Fm(0)p 2825 1984 79 4 v 2843 2060 a Ft(2)2913
79630 < 2003 y([)p Fi(s)p Ft(\()p Fi(r)3044 2015 y Fh(ij)3103
79631 < 2003 y Ft(\))p Fi(w)r Ft(\()p Fg(r)3267 2015 y Fh(ij)3327
79632 < 2003 y Fi(;)14 b Fg(\012)3433 2015 y Fh(i)3461 2003 y
79633 < Fi(;)g Fg(\012)3567 2015 y Fh(j)3602 2003 y Ft(\)])2833
79634 < 2212 y(+)2926 2156 y Fi(\027)2972 2126 y Fs(0)2967 2176
79635 < y Fm(0)p 2926 2193 V 2945 2269 a Ft(2)3015 2212 y([)p
79636 < Fi(s)3077 2178 y Fs(0)3100 2212 y Ft(\()p Fi(r)3169 2224
79637 < y Fh(ij)3228 2212 y Ft(\))p Fi(w)3321 2178 y Fs(0)3345
79638 < 2212 y Ft(\()p Fg(r)3416 2224 y Fh(ij)3475 2212 y Fi(;)g
79639 < Fg(\012)3581 2224 y Fh(i)3609 2212 y Fi(;)g Fg(\012)3715
79640 < 2224 y Fh(j)3750 2212 y Ft(\)])p Fi(;)3937 2111 y Ft(\(10\))2125
79641 < 2418 y(where)27 b Fi(\027)2406 2430 y Fm(0)2471 2418
79642 < y Ft(scales)f(the)i(strength)f(of)g(the)h(tetrahedral)e(attrac-)2042
79643 < 2513 y(tion)40 b(and)g Fi(\027)2445 2483 y Fs(0)2440
79644 < 2534 y Fm(0)2517 2513 y Ft(acts)g(in)g(an)g(iden)n(tical)g(fashion)g
79645 < (on)g(the)g(dip)r(ole)2042 2609 y(repulsion)29 b(term.)43
79625 > 3076 y Fj(u)2198 3036 y Fi(sp)2198 3099 y(ij)2267 3076
79626 > y Fu(\()p Fh(r)2338 3088 y Fi(ij)2398 3076 y Fj(;)14
79627 > b Fh(\012)2503 3088 y Fi(i)2531 3076 y Fj(;)g Fh(\012)2637
79628 > 3088 y Fi(j)2672 3076 y Fu(\))23 b(=)2825 3020 y Fj(\027)2866
79629 > 3032 y Fn(0)p 2825 3057 79 4 v 2843 3133 a Fu(2)2913
79630 > 3076 y([)p Fj(s)p Fu(\()p Fj(r)3044 3088 y Fi(ij)3103
79631 > 3076 y Fu(\))p Fj(w)r Fu(\()p Fh(r)3267 3088 y Fi(ij)3327
79632 > 3076 y Fj(;)14 b Fh(\012)3433 3088 y Fi(i)3461 3076 y
79633 > Fj(;)g Fh(\012)3567 3088 y Fi(j)3602 3076 y Fu(\)])2833
79634 > 3285 y(+)2926 3229 y Fj(\027)2972 3199 y Ft(0)2967 3249
79635 > y Fn(0)p 2926 3266 V 2945 3342 a Fu(2)3015 3285 y([)p
79636 > Fj(s)3077 3251 y Ft(0)3100 3285 y Fu(\()p Fj(r)3169 3297
79637 > y Fi(ij)3228 3285 y Fu(\))p Fj(w)3321 3251 y Ft(0)3345
79638 > 3285 y Fu(\()p Fh(r)3416 3297 y Fi(ij)3475 3285 y Fj(;)g
79639 > Fh(\012)3581 3297 y Fi(i)3609 3285 y Fj(;)g Fh(\012)3715
79640 > 3297 y Fi(j)3750 3285 y Fu(\)])p Fj(;)3937 3184 y Fu(\(10\))2125
79641 > 3491 y(where)27 b Fj(\027)2406 3503 y Fn(0)2471 3491
79642 > y Fu(scales)f(the)i(strength)f(of)g(the)h(tetrahedral)e(attrac-)2042
79643 > 3586 y(tion)40 b(and)g Fj(\027)2445 3556 y Ft(0)2440
79644 > 3607 y Fn(0)2517 3586 y Fu(acts)g(in)g(an)g(iden)n(tical)g(fashion)g
79645 > (on)g(the)g(dip)r(ole)2042 3682 y(repulsion)29 b(term.)43
79646   b(F)-7 b(or)30 b(purp)r(oses)f(of)h(the)g(reparameterization,)2042
79647 < 2704 y(the)j(separation)e(w)n(as)g(p)r(erformed,)i(but)h(the)f(\014nal)
79648 < f(parameters)2042 2800 y(w)n(ere)h(adjusted)i(so)f(that)h(it)g(is)f
79649 < (unnecessary)f(to)i(separate)e(the)2042 2895 y(terms)25
79647 > 3777 y(the)j(separation)e(w)n(as)g(p)r(erformed,)i(but)h(the)f(\014nal)
79648 > f(parameters)2042 3873 y(w)n(ere)h(adjusted)i(so)f(that)h(it)g(is)f
79649 > (unnecessary)f(to)i(separate)e(the)2042 3968 y(terms)25
79650   b(when)i(implemen)n(ting)f(the)g(adjusted)h(w)n(ater)d(p)r(oten)n
79651 < (tials.)2042 2991 y(The)e(results)g(of)h(the)g(reparameterizations)c
79652 < (are)j(sho)n(wn)f(in)i(table)2042 3086 y(I.)60 b(Note)35
79651 > (tials.)2042 4064 y(The)e(results)g(of)h(the)g(reparameterizations)c
79652 > (are)j(sho)n(wn)f(in)i(table)2042 4159 y(I.)60 b(Note)35
79653   b(that)h(b)r(oth)f(the)h(tetrahedral)e(attractiv)n(e)g(and)h(dip)r(o-)
79654 < 2042 3182 y(lar)k(repulsiv)n(e)g(don't)h(share)f(the)h(same)g(lo)n(w)n
79655 < (er)e(cuto\013)i(\()p Fi(r)3916 3194 y Fh(l)3943 3182
79656 < y Ft(\))g(in)2042 3277 y(the)d(newly)g(parameterized)f(p)r(oten)n
79657 < (tials)h(-)f(soft)i(stic)n(ky)e(dip)r(ole)2042 3373 y(enhanced)f
79658 < (\(SSD/E\))h(and)f(soft)h(stic)n(ky)f(dip)r(ole)g(reaction)g(\014eld)
79659 < 2042 3468 y(\(SSD/RF\).)2125 3564 y(In)20 b(the)g(pap)r(er)f(detailing)
79660 < h(the)g(dev)n(elopmen)n(t)f(of)h(SSD,)g(Liu)g(and)2042
79661 < 3659 y(Ic)n(hiy)n(e)h(placed)g(particular)g(emphasis)g(on)h(an)f
79662 < (accurate)g(descrip-)2042 3755 y(tion)29 b(of)f(the)i(\014rst)e(solv)-5
79663 < b(ation)28 b(shell.)40 b(This)29 b(resulted)g(in)g(a)f(some-)2042
79664 < 3850 y(what)40 b(tall)f(and)h(sharp)f(\014rst)h(p)r(eak)f(that)i(in)n
79665 < (tegrated)d(to)i(giv)n(e)2042 3945 y(similar)35 b(co)r(ordination)g(n)n
79666 < (um)n(b)r(ers)g(to)h(the)g(exp)r(erimen)n(tal)g(data)2042
79667 < 4041 y(obtained)26 b(b)n(y)g(Sop)r(er)f(and)h(Phillips.)3184
79668 < 4011 y Fm(5,24)3333 4041 y Ft(New)g(exp)r(erimen)n(tal)g(x-)2042
79669 < 4136 y(ra)n(y)i(scattering)h(data)g(from)h(the)g(Head-Gordon)e(lab)h
79670 < (indicates)2042 4232 y(a)j(sligh)n(tly)f(lo)n(w)n(er)g(and)h(shifted)h
79671 < (\014rst)f(p)r(eak)f(in)i(the)f(g)3743 4244 y Fm(OO)3849
79672 < 4232 y Ft(\()p Fi(r)r Ft(\),)j(so)2042 4327 y(adjustmen)n(ts)25
79673 < b(to)h(SSD)g(w)n(ere)e(made)h(while)h(taking)f(in)n(to)g(consid-)2042
79674 < 4423 y(eration)i(the)i(new)g(exp)r(erimen)n(tal)f(\014ndings.)3442
79675 < 4393 y Fm(23)3540 4423 y Ft(Figure)g(7)g(sho)n(ws)2042
79651 < 4518 y(the)23 b(relo)r(cation)f(of)i(the)f(\014rst)g(p)r(eak)g(of)h
79652 < (the)f(o)n(xygen-o)n(xygen)d(g\()p Fl(r)9 b Ft(\))2042
79653 < 4614 y(b)n(y)30 b(comparing)g(the)h(original)f(SSD)i(\(with)f(and)g
79654 < (without)h(reac-)2042 4709 y(tion)24 b(\014eld\),)i(SSD-E,)e(and)g
79655 < (SSD-RF)h(to)g(the)f(new)h(exp)r(erimen)n(tal)2042 4805
79656 < y(results.)71 b(Both)39 b(the)g(mo)r(di\014ed)h(w)n(ater)e(mo)r(dels)h
79657 < (ha)n(v)n(e)f(shorter)2042 4900 y(p)r(eaks)23 b(that)h(are)f(brough)n
79658 < (t)f(in)i(more)f(closely)g(to)h(the)g(exp)r(erimen-)2042
79659 < 4996 y(tal)33 b(p)r(eak)g(\(as)h(seen)f(in)h(the)f(insets)h(of)f
79660 < (\014gure)g(7\).)54 b(This)34 b(struc-)2042 5091 y(tural)c(alteration)g
79661 < (w)n(as)g(accomplished)h(b)n(y)f(a)h(reduction)g(in)g(the)2042
79662 < 5187 y(Lennard-Jones)k Fi(\033)41 b Ft(v)-5 b(ariable)37
79663 < b(as)g(w)n(ell)g(as)g(adjustmen)n(t)h(of)g(the)2042 5282
79664 < y(stic)n(ky)25 b(p)r(oten)n(tial)h(strength)f(and)h(cuto\013s.)37
79665 < b(The)25 b(cuto\013s)h(for)g(the)2042 5378 y(tetrahedral)34
79666 < b(attractiv)n(e)g(and)i(dip)r(olar)e(repulsiv)n(e)h(terms)g(w)n(ere)p
79667 < eop
79654 > 2042 4255 y(lar)k(repulsiv)n(e)g(don't)h(share)f(the)h(same)g(lo)n(w)n
79655 > (er)e(cuto\013)i(\()p Fj(r)3916 4267 y Fi(l)3943 4255
79656 > y Fu(\))g(in)2042 4350 y(the)d(newly)g(parameterized)f(p)r(oten)n
79657 > (tials)h(-)f(soft)i(stic)n(ky)e(dip)r(ole)2042 4446 y(enhanced)f
79658 > (\(SSD/E\))h(and)f(soft)h(stic)n(ky)f(dip)r(ole)g(reaction)g(\014eld)
79659 > 2042 4541 y(\(SSD/RF\).)2125 4636 y(In)20 b(the)g(pap)r(er)f(detailing)
79660 > h(the)g(dev)n(elopmen)n(t)f(of)h(SSD,)g(Liu)g(and)2042
79661 > 4732 y(Ic)n(hiy)n(e)h(placed)g(particular)g(emphasis)g(on)h(an)f
79662 > (accurate)g(descrip-)2042 4827 y(tion)29 b(of)f(the)i(\014rst)e(solv)-5
79663 > b(ation)28 b(shell.)40 b(This)29 b(resulted)g(in)g(a)f(some-)2042
79664 > 4923 y(what)40 b(tall)f(and)h(sharp)f(\014rst)h(p)r(eak)f(that)i(in)n
79665 > (tegrated)d(to)i(giv)n(e)2042 5018 y(similar)35 b(co)r(ordination)g(n)n
79666 > (um)n(b)r(ers)g(to)h(the)g(exp)r(erimen)n(tal)g(data)2042
79667 > 5114 y(obtained)26 b(b)n(y)g(Sop)r(er)f(and)h(Phillips.)3184
79668 > 5084 y Fn(5,25)3333 5114 y Fu(New)g(exp)r(erimen)n(tal)g(x-)2042
79669 > 5209 y(ra)n(y)i(scattering)h(data)g(from)h(the)g(Head-Gordon)e(lab)h
79670 > (indicates)2042 5305 y(a)j(sligh)n(tly)f(lo)n(w)n(er)g(and)h(shifted)h
79671 > (\014rst)f(p)r(eak)f(in)i(the)f(g)3743 5317 y Fn(OO)3849
79672 > 5305 y Fu(\()p Fj(r)r Fu(\),)j(so)2042 5400 y(adjustmen)n(ts)25
79673 > b(to)h(SSD)g(w)n(ere)e(made)h(while)h(taking)f(in)n(to)g(consid-)2042
79674 > 5496 y(eration)i(the)i(new)g(exp)r(erimen)n(tal)f(\014ndings.)3442
79675 > 5466 y Fn(24)3540 5496 y Fu(Figure)g(7)g(sho)n(ws)p eop
79676   %%Page: 7 7
79677 < 7 6 bop 4043 -299 a Ft(7)-133 2930 y @beginspecial 71
79677 > 7 6 bop 4043 -299 a Fu(7)-133 2930 y @beginspecial 71
79678   @llx 60 @lly 514 @urx 743 @ury 2409 @rwi @setspecial
79679   %%BeginDocument: gofrCompare.epsi
79680   %!PS-Adobe-2.0 EPSF-1.2
# Line 94611 | Line 94619 | cleartomark countdictstack exch sub { end } repeat res
94619   %%EOF
94620  
94621   %%EndDocument
94622 < @endspecial -150 3100 a Fq(FIG.)26 b(7:)34 b(Plots)27
94623 < b(comparing)e(exp)r(erimen)n(t)1076 3068 y Fc(23)1165
94624 < 3100 y Fq(with)g(SSD/E)g(and)g(SSD)-150 3187 y(without)c(reaction)g
94622 > @endspecial -150 3100 a Fr(FIG.)26 b(7:)34 b(Plots)27
94623 > b(comparing)e(exp)r(erimen)n(t)1076 3068 y Fc(24)1165
94624 > 3100 y Fr(with)g(SSD/E)g(and)g(SSD)-150 3187 y(without)c(reaction)g
94625   (\014eld)g(\(top\),)g(as)h(w)n(ell)f(as)h(SSD/RF)d(and)h(SSD)g(with)
94626   -150 3274 y(reaction)34 b(\014eld)f(turned)f(on)h(\(b)r(ottom\).)56
94627   b(The)33 b(insets)h(sho)n(w)g(the)f(re-)-150 3361 y(sp)r(ectiv)n(e)23
# Line 488661 | Line 488669 | b(Ligh)n(t)37 b(areas)i(corresp)r(ond)e(to)h(the)-150
488669   b(Ligh)n(t)37 b(areas)i(corresp)r(ond)e(to)h(the)-150
488670   5144 y(tetrahedral)29 b(attractiv)n(e)h(part,)g(and)e(the)h(dark)n(er)g
488671   (areas)h(corresp)r(ond)-150 5231 y(to)c(the)f(dip)r(olar)i(repulsiv)n
488672 < (e)e(part.)2042 -83 y Ft(nearly)f(sw)n(app)r(ed)h(with)h(eac)n(h)f
488673 < (other.)36 b(Isosurfaces)23 b(of)j(the)g(origi-)2042
488674 < 12 y(nal)h(and)g(mo)r(di\014ed)h(stic)n(ky)f(p)r(oten)n(tials)h(are)e
488675 < (sho)n(wn)h(in)h(\014gure)3993 -18 y Fb(?)4061 12 y Ft(.)2042
488676 < 108 y(In)22 b(these)h(isosurfaces,)f(it)h(is)f(easy)f(to)i(see)f(ho)n
488677 < (w)g(altering)f(the)i(cut-)2042 203 y(o\013s)i(c)n(hanges)f(the)i
488678 < (repulsiv)n(e)e(and)i(attractiv)n(e)e(c)n(haracter)f(of)j(the)2042
488679 < 299 y(particles.)53 b(With)34 b(a)f(reduced)g(repulsiv)n(e)g(surface)f
488680 < (\(the)i(dark)n(er)2042 394 y(region\),)25 b(the)h(particles)g(can)f
488681 < (mo)n(v)n(e)g(closer)g(to)g(one)h(another,)f(in-)2042
488682 < 490 y(creasing)i(the)j(densit)n(y)e(for)h(the)g(o)n(v)n(erall)e
488683 < (system.)41 b(This)29 b(c)n(hange)2042 585 y(in)d(in)n(teraction)e
488672 > (e)e(part.)2042 -83 y Fu(the)e(relo)r(cation)f(of)i(the)f(\014rst)g(p)r
488673 > (eak)g(of)h(the)f(o)n(xygen-o)n(xygen)d(g\()p Fm(r)9
488674 > b Fu(\))2042 12 y(b)n(y)30 b(comparing)g(the)h(original)f(SSD)i(\(with)
488675 > f(and)g(without)h(reac-)2042 108 y(tion)24 b(\014eld\),)i(SSD-E,)e(and)
488676 > g(SSD-RF)h(to)g(the)f(new)h(exp)r(erimen)n(tal)2042 203
488677 > y(results.)71 b(Both)39 b(the)g(mo)r(di\014ed)h(w)n(ater)e(mo)r(dels)h
488678 > (ha)n(v)n(e)f(shorter)2042 299 y(p)r(eaks)23 b(that)h(are)f(brough)n(t)
488679 > f(in)i(more)f(closely)g(to)h(the)g(exp)r(erimen-)2042
488680 > 394 y(tal)33 b(p)r(eak)g(\(as)h(seen)f(in)h(the)f(insets)h(of)f
488681 > (\014gure)g(7\).)54 b(This)34 b(struc-)2042 490 y(tural)c(alteration)g
488682 > (w)n(as)g(accomplished)h(b)n(y)f(a)h(reduction)g(in)g(the)2042
488683 > 585 y(Lennard-Jones)k Fj(\033)41 b Fu(v)-5 b(ariable)37
488684 > b(as)g(w)n(ell)g(as)g(adjustmen)n(t)h(of)g(the)2042 681
488685 > y(stic)n(ky)25 b(p)r(oten)n(tial)h(strength)f(and)h(cuto\013s.)37
488686 > b(The)25 b(cuto\013s)h(for)g(the)2042 776 y(tetrahedral)34
488687 > b(attractiv)n(e)g(and)i(dip)r(olar)e(repulsiv)n(e)h(terms)g(w)n(ere)
488688 > 2042 872 y(nearly)24 b(sw)n(app)r(ed)h(with)h(eac)n(h)f(other.)36
488689 > b(Isosurfaces)23 b(of)j(the)g(origi-)2042 967 y(nal)h(and)g(mo)r
488690 > (di\014ed)h(stic)n(ky)f(p)r(oten)n(tials)h(are)e(sho)n(wn)h(in)h
488691 > (\014gure)3993 937 y Fb(?)4061 967 y Fu(.)2042 1063 y(In)22
488692 > b(these)h(isosurfaces,)f(it)h(is)f(easy)f(to)i(see)f(ho)n(w)g(altering)
488693 > f(the)i(cut-)2042 1158 y(o\013s)i(c)n(hanges)f(the)i(repulsiv)n(e)e
488694 > (and)i(attractiv)n(e)e(c)n(haracter)f(of)j(the)2042 1254
488695 > y(particles.)53 b(With)34 b(a)f(reduced)g(repulsiv)n(e)g(surface)f
488696 > (\(the)i(dark)n(er)2042 1349 y(region\),)25 b(the)h(particles)g(can)f
488697 > (mo)n(v)n(e)g(closer)g(to)g(one)h(another,)f(in-)2042
488698 > 1445 y(creasing)i(the)j(densit)n(y)e(for)h(the)g(o)n(v)n(erall)e
488699 > (system.)41 b(This)29 b(c)n(hange)2042 1540 y(in)d(in)n(teraction)e
488700   (cuto\013)i(also)f(results)g(in)h(a)f(more)g(gradual)f(orien-)2042
488701 < 681 y(tational)c(motion)g(b)n(y)g(allo)n(wing)f(the)i(particles)f(to)g
488702 < (main)n(tain)g(pre-)2042 776 y(ferred)k(dip)r(olar)g(arrangemen)n(ts)f
488703 < (b)r(efore)i(they)g(b)r(egin)g(to)g(feel)g(the)2042 872
488701 > 1636 y(tational)c(motion)g(b)n(y)g(allo)n(wing)f(the)i(particles)f(to)g
488702 > (main)n(tain)g(pre-)2042 1731 y(ferred)k(dip)r(olar)g(arrangemen)n(ts)f
488703 > (b)r(efore)i(they)g(b)r(egin)g(to)g(feel)g(the)2042 1826
488704   y(pull)c(of)g(the)g(tetrahedral)f(restructuring.)33 b(Up)r(on)22
488705 < b(mo)n(ving)d(closer)2042 967 y(together,)28 b(the)h(dip)r(olar)e
488705 > b(mo)n(ving)d(closer)2042 1922 y(together,)28 b(the)h(dip)r(olar)e
488706   (repulsion)h(term)g(b)r(ecomes)h(activ)n(e)e(and)2042
488707 < 1063 y(excludes)39 b(the)h(unph)n(ysical)f(arrangemen)n(ts.)70
488708 < b(This)40 b(compares)2042 1158 y(with)25 b(the)g(original)e(SSD's)i
488707 > 2017 y(excludes)39 b(the)h(unph)n(ysical)f(arrangemen)n(ts.)70
488708 > b(This)40 b(compares)2042 2113 y(with)25 b(the)g(original)e(SSD's)i
488709   (excluding)f(dip)r(olar)g(b)r(efore)g(the)h(par-)2042
488710 < 1254 y(ticles)k(feel)h(the)f(pull)h(of)f(the)h(\\h)n(ydrogen)d(b)r
488711 < (onds".)41 b(Aside)30 b(from)2042 1349 y(impro)n(ving)35
488710 > 2208 y(ticles)k(feel)h(the)f(pull)h(of)f(the)h(\\h)n(ydrogen)d(b)r
488711 > (onds".)41 b(Aside)30 b(from)2042 2304 y(impro)n(ving)35
488712   b(the)i(shap)r(e)f(of)h(the)g(\014rst)f(p)r(eak)g(in)h(the)g(g\()p
488713 < Fl(r)9 b Ft(\),)39 b(this)2042 1445 y(impro)n(v)n(es)27
488713 > Fm(r)9 b Fu(\),)39 b(this)2042 2399 y(impro)n(v)n(es)27
488714   b(the)h(densities)h(considerably)e(b)n(y)h(allo)n(wing)f(the)i(p)r(er-)
488715 < 2042 1540 y(sistence)j(of)g(full)g(dip)r(olar)g(c)n(haracter)e(b)r(elo)
488716 < n(w)i(the)g(previous)f(4.0)2042 1621 y(\027)2042 1636
488717 < y(A)d(cuto\013.)2125 1731 y(While)43 b(adjusting)f(the)h(lo)r(cation)f
488718 < (and)h(shap)r(e)f(of)h(the)f(\014rst)2042 1826 y(p)r(eak)23
488719 < b(of)h(g\()p Fl(r)9 b Ft(\))24 b(impro)n(v)n(es)e(the)i(densities)g(to)
488720 < f(some)h(degree,)f(these)2042 1922 y(c)n(hanges)34 b(alone)i(are)f
488715 > 2042 2495 y(sistence)j(of)g(full)g(dip)r(olar)g(c)n(haracter)e(b)r(elo)
488716 > n(w)i(the)g(previous)f(4.0)2042 2575 y(\027)2042 2590
488717 > y(A)d(cuto\013.)2125 2686 y(While)43 b(adjusting)f(the)h(lo)r(cation)f
488718 > (and)h(shap)r(e)f(of)h(the)f(\014rst)2042 2781 y(p)r(eak)23
488719 > b(of)h(g\()p Fm(r)9 b Fu(\))24 b(impro)n(v)n(es)e(the)i(densities)g(to)
488720 > f(some)h(degree,)f(these)2042 2877 y(c)n(hanges)34 b(alone)i(are)f
488721   (insu\016cien)n(t)h(to)g(bring)g(the)g(system)g(den-)2042
488722 < 2017 y(sities)c(up)h(to)g(the)g(v)-5 b(alues)32 b(observ)n(ed)f(exp)r
488722 > 2972 y(sities)c(up)h(to)g(the)g(v)-5 b(alues)32 b(observ)n(ed)f(exp)r
488723   (erimen)n(tally)-7 b(.)51 b(T)-7 b(o)32 b(\014n-)2042
488724 < 2113 y(ish)i(bringing)f(up)i(the)f(densities,)i(the)f(dip)r(ole)f
488725 < (momen)n(ts)g(w)n(ere)2042 2208 y(increased)g(in)h(b)r(oth)h(the)g
488724 > 3068 y(ish)i(bringing)f(up)i(the)f(densities,)i(the)f(dip)r(ole)f
488725 > (momen)n(ts)g(w)n(ere)2042 3163 y(increased)g(in)h(b)r(oth)h(the)g
488726   (adjusted)f(mo)r(dels.)60 b(Being)35 b(a)g(dip)r(ole)2042
488727 < 2304 y(based)e(mo)r(del,)i(the)f(structure)f(and)g(transp)r(ort)g(are)f
488728 < (v)n(ery)h(sen-)2042 2399 y(sitiv)n(e)40 b(to)h(c)n(hanges)f(in)h(the)h
488729 < (dip)r(ole)f(momen)n(t.)77 b(The)41 b(original)2042 2495
488727 > 3259 y(based)e(mo)r(del,)i(the)f(structure)f(and)g(transp)r(ort)g(are)f
488728 > (v)n(ery)h(sen-)2042 3354 y(sitiv)n(e)40 b(to)h(c)n(hanges)f(in)h(the)h
488729 > (dip)r(ole)f(momen)n(t.)77 b(The)41 b(original)2042 3450
488730   y(SSD)27 b(simply)f(used)h(the)f(dip)r(ole)h(momen)n(t)f(calculated)g
488731 < (from)g(the)2042 2590 y(TIP3P)44 b(w)n(ater)h(mo)r(del,)50
488731 > (from)g(the)2042 3545 y(TIP3P)44 b(w)n(ater)h(mo)r(del,)50
488732   b(whic)n(h)c(at)f(2.35)f(D)j(is)e(signi\014can)n(tly)2042
488733 < 2686 y(greater)24 b(than)h(the)h(exp)r(erimen)n(tal)g(gas)e(phase)h(v)
488734 < -5 b(alue)26 b(of)f(1.84)g(D.)2042 2781 y(The)33 b(larger)e(dip)r(ole)j
488733 > 3641 y(greater)24 b(than)h(the)h(exp)r(erimen)n(tal)g(gas)e(phase)h(v)
488734 > -5 b(alue)26 b(of)f(1.84)g(D.)2042 3736 y(The)33 b(larger)e(dip)r(ole)j
488735   (momen)n(t)f(is)g(a)g(more)f(realistic)g(v)-5 b(alue)33
488736 < b(and)2042 2877 y(impro)n(v)n(e)24 b(the)i(dielectric)g(prop)r(erties)f
488737 < (of)h(the)g(\015uid.)37 b(Both)26 b(theo-)2042 2972 y(retical)h(and)i
488736 > b(and)2042 3831 y(impro)n(v)n(e)24 b(the)i(dielectric)g(prop)r(erties)f
488737 > (of)h(the)g(\015uid.)37 b(Both)26 b(theo-)2042 3927 y(retical)h(and)i
488738   (exp)r(erimen)n(tal)e(measuremen)n(ts)h(indicate)g(a)g(liquid)2042
488739 < 3068 y(phase)18 b(dip)r(ole)i(momen)n(t)f(ranging)e(from)i(2.4)f(D)i
488740 < (to)f(v)-5 b(alues)19 b(as)f(high)2042 3163 y(as)29 b(3.11)g(D,)i(so)e
488739 > 4022 y(phase)18 b(dip)r(ole)i(momen)n(t)f(ranging)e(from)i(2.4)f(D)i
488740 > (to)f(v)-5 b(alues)19 b(as)f(high)2042 4118 y(as)29 b(3.11)g(D,)i(so)e
488741   (there)h(is)g(quite)g(a)g(range)f(a)n(v)-5 b(ailable)29
488742 < b(for)g(adjust-)2042 3259 y(ing)c(the)i(dip)r(ole)e(momen)n(t.)2880
488743 < 3228 y Fm(25)q({28)3076 3259 y Ft(The)h(increasing)e(of)i(the)g(dip)r
488744 < (ole)2042 3354 y(momen)n(ts)34 b(to)g(2.418)f(and)h(2.48)f(D)i(for)e
488745 < (SSD/E)h(and)h(SSD/RF)2042 3450 y(resp)r(ectiv)n(ely)c(is)g(mo)r
488742 > b(for)g(adjust-)2042 4213 y(ing)c(the)i(dip)r(ole)e(momen)n(t.)2880
488743 > 4183 y Fn(26)q({29)3076 4213 y Fu(The)h(increasing)e(of)i(the)g(dip)r
488744 > (ole)2042 4309 y(momen)n(ts)34 b(to)g(2.418)f(and)h(2.48)f(D)i(for)e
488745 > (SSD/E)h(and)h(SSD/RF)2042 4404 y(resp)r(ectiv)n(ely)c(is)g(mo)r
488746   (derate)h(in)g(the)g(range)f(of)g(the)i(exp)r(erimen-)2042
488747 < 3545 y(tal)27 b(v)-5 b(alues;)27 b(ho)n(w)n(ev)n(er,)f(it)i(leads)f(to)
488748 < g(signi\014can)n(t)g(c)n(hanges)f(in)i(the)2042 3641
488747 > 4500 y(tal)27 b(v)-5 b(alues;)27 b(ho)n(w)n(ev)n(er,)f(it)i(leads)f(to)
488748 > g(signi\014can)n(t)g(c)n(hanges)f(in)i(the)2042 4595
488749   y(densit)n(y)f(and)h(transp)r(ort)e(of)i(the)g(w)n(ater)e(mo)r(dels.)
488750 < 2125 3736 y(In)31 b(order)e(to)i(demonstrate)f(the)i(b)r(ene\014ts)f
488751 < (of)g(this)g(reparam-)2042 3831 y(eterization,)i(a)g(series)f(of)h(NPT)
488752 < g(and)g(NVE)g(sim)n(ulations)f(w)n(ere)2042 3927 y(p)r(erformed)25
488750 > 2125 4691 y(In)31 b(order)e(to)i(demonstrate)f(the)i(b)r(ene\014ts)f
488751 > (of)g(this)g(reparam-)2042 4786 y(eterization,)i(a)g(series)f(of)h(NPT)
488752 > g(and)g(NVE)g(sim)n(ulations)f(w)n(ere)2042 4882 y(p)r(erformed)25
488753   b(to)h(prob)r(e)g(the)g(densit)n(y)g(and)g(transp)r(ort)f(prop)r
488754 < (erties)2042 4022 y(of)37 b(the)h(adapted)f(mo)r(dels)h(and)f(compare)f
488755 < (the)i(results)f(to)h(the)2042 4118 y(original)26 b(SSD)j(mo)r(del.)37
488754 > (erties)2042 4977 y(of)37 b(the)h(adapted)f(mo)r(dels)h(and)f(compare)f
488755 > (the)i(results)f(to)h(the)2042 5073 y(original)26 b(SSD)j(mo)r(del.)37
488756   b(This)28 b(comparison)e(in)n(v)n(olv)n(ed)h(full)h(NPT)2042
488757 < 4213 y(melting)f(sequences)f(for)g(b)r(oth)i(SSD/E)e(and)h(SSD/RF,)g
488758 < (as)f(w)n(ell)2042 4309 y(as)19 b(NVE)i(transp)r(ort)e(calculations)g
488759 < (at)h(b)r(oth)h(self-consisten)n(t)e(and)2042 4404 y(exp)r(erimen)n
488757 > 5168 y(melting)f(sequences)f(for)g(b)r(oth)i(SSD/E)e(and)h(SSD/RF,)g
488758 > (as)f(w)n(ell)2042 5264 y(as)19 b(NVE)i(transp)r(ort)e(calculations)g
488759 > (at)h(b)r(oth)h(self-consisten)n(t)e(and)2042 5359 y(exp)r(erimen)n
488760   (tal)j(densities.)35 b(Again,)24 b(the)f(results)g(come)f(from)h(\014v)
488761 < n(e)2042 4500 y(separate)37 b(sim)n(ulations)h(of)h(1024)e(particle)h
488738 < (systems,)j(and)e(the)2042 4595 y(melting)23 b(sequences)f(w)n(ere)g
488739 < (started)g(from)h(di\013eren)n(t)g(ice)g Fi(I)3844 4607
488740 < y Fh(h)3910 4595 y Ft(crys-)2042 4691 y(tals)30 b(constructed)f(as)h
488741 < (stated)g(previously)-7 b(.)44 b(Lik)n(e)30 b(b)r(efore,)g(all)g(of)
488742 < 2042 4786 y(the)e(NPT)f(sim)n(ulations)f(w)n(ere)h(equilibrated)f(for)h
488743 < (100)f(ps)h(b)r(efore)2042 4882 y(a)36 b(200)f(ps)h(data)g(collection)g
488744 < (run,)i(and)e(they)h(used)f(the)h(previ-)2042 4977 y(ous)25
488745 < b(temp)r(erature's)g(\014nal)g(con\014guration)f(as)g(a)h(starting)g(p)
488746 < r(oin)n(t.)2042 5073 y(All)e(of)g(the)g(NVE)g(sim)n(ulations)f(had)h
488747 < (the)g(same)f(thermalization,)2042 5168 y(equilibration,)30
488748 < b(and)g(data)f(collection)h(times)g(stated)g(earlier)f(in)2042
488749 < 5264 y(this)f(pap)r(er.)2125 5359 y(Figure)i(9)g(sho)n(ws)g(the)h
488750 < (densit)n(y)f(pro\014le)h(for)f(the)h(SSD/E)f(w)n(a-)p
488751 < eop
488761 > n(e)p eop
488762   %%Page: 8 8
488763 < 8 7 bop 4043 -299 a Ft(8)-133 2245 y @beginspecial 44
488763 > 8 7 bop 4043 -299 a Fu(8)-133 2245 y @beginspecial 44
488764   @llx 93 @lly 517 @urx 661 @ury 2409 @rwi @setspecial
488765   %%BeginDocument: ssdecompare.epsi
488766   %!PS-Adobe-2.0 EPSF-1.2
# Line 497244 | Line 497254 | cleartomark countdictstack exch sub { end } repeat res
497254   %%EOF
497255  
497256   %%EndDocument
497257 < @endspecial -150 2415 a Fq(FIG.)34 b(9:)50 b(Comparison)34
497257 > @endspecial -150 2415 a Fr(FIG.)34 b(9:)50 b(Comparison)34
497258   b(of)h(densities)f(calculated)g(with)g(SSD/E)f(to)-150
497259   2502 y(SSD)c(without)i(a)g(reaction)g(\014eld,)h(TIP4P)1102
497260 < 2471 y Fc(18)1168 2502 y Fq(,)g(TIP3P)1446 2471 y Fc(18)1512
497261 < 2502 y Fq(,)g(SPC/E)1805 2471 y Fc(19)1871 2502 y Fq(,)-150
497262 < 2590 y(and)e(Exp)r(erimen)n(t)397 2558 y Fc(20)461 2590
497263 < y Fq(.)49 b(The)31 b(upp)r(er)f(plot)g(includes)h(error)g(bars,)i(and)
497260 > 2471 y Fc(19)1168 2502 y Fr(,)g(TIP3P)1446 2471 y Fc(19)1512
497261 > 2502 y Fr(,)g(SPC/E)1805 2471 y Fc(20)1871 2502 y Fr(,)-150
497262 > 2590 y(and)e(Exp)r(erimen)n(t)397 2558 y Fc(21)461 2590
497263 > y Fr(.)49 b(The)31 b(upp)r(er)f(plot)g(includes)h(error)g(bars,)i(and)
497264   -150 2677 y(the)23 b(calculated)h(results)f(from)g(the)g(other)g
497265   (references)h(w)n(ere)g(remo)n(v)n(ed)-150 2764 y(for)i(clarit)n(y)-6
497266 < b(.)-150 3044 y Ft(ter)33 b(mo)r(del)h(in)f(comparison)f(to)h(the)h
497267 < (original)e(SSD)i(without)g(a)-150 3140 y(reaction)k(\014eld,)k(exp)r
497268 < (erimen)n(t,)g(and)d(the)g(other)g(common)g(w)n(a-)-150
497269 < 3235 y(ter)f(mo)r(dels)g(considered)f(previously)-7 b(.)68
497270 < b(The)38 b(calculated)g(den-)-150 3331 y(sities)c(ha)n(v)n(e)e
497271 < (increased)h(signi\014can)n(tly)g(o)n(v)n(er)f(the)i(original)f(SSD)
497272 < -150 3426 y(mo)r(del)28 b(and)h(matc)n(h)f(the)g(exp)r(erimen)n(tal)g
497273 < (v)-5 b(alue)28 b(just)h(b)r(elo)n(w)f(298)-150 3522
497274 < y(K.)20 b(A)n(t)h(298)f(K,)g(the)h(densit)n(y)g(of)f(SSD/E)h(is)f
497275 < (0.995)p Fe(\006)p Ft(0.001)d(g/cm)1833 3491 y Fm(3)1869
497276 < 3522 y Ft(,)-150 3617 y(whic)n(h)k(compares)e(w)n(ell)h(with)i(the)f
497277 < (exp)r(erimen)n(tal)f(v)-5 b(alue)21 b(of)f(0.997)-150
497278 < 3713 y(g/cm)40 3682 y Fm(3)118 3713 y Ft(and)41 b(is)h(considerably)e
497279 < (b)r(etter)i(than)f(the)h(SSD)h(v)-5 b(alue)-150 3808
497280 < y(of)43 b(0.967)p Fe(\006)p Ft(0.003)38 b(g/cm)635 3778
497281 < y Fm(3)671 3808 y Ft(.)82 b(The)43 b(increased)f(dip)r(ole)g(momen)n(t)
497282 < -150 3903 y(in)33 b(SSD/E)f(has)f(help)r(ed)i(to)f(\015atten)h(out)f
497283 < (the)h(curv)n(e)e(at)h(higher)-150 3999 y(temp)r(eratures,)25
497284 < b(only)g(the)h(impro)n(v)n(emen)n(t)e(is)i(marginal)e(at)h(b)r(est.)
497285 < -150 4094 y(This)30 b(steep)f(drop)h(in)f(densities)h(is)g(due)g(to)f
497286 < (the)h(dip)r(olar)f(rather)-150 4190 y(than)24 b(c)n(harge)e(based)i
497266 > b(.)-150 3044 y Fu(separate)37 b(sim)n(ulations)h(of)h(1024)e(particle)
497267 > h(systems,)j(and)e(the)-150 3140 y(melting)23 b(sequences)f(w)n(ere)g
497268 > (started)h(from)f(di\013eren)n(t)h(ice)g Fj(I)1652 3152
497269 > y Fi(h)1719 3140 y Fu(crys-)-150 3235 y(tals)30 b(constructed)g(as)f
497270 > (stated)h(previously)-7 b(.)44 b(Lik)n(e)30 b(b)r(efore,)g(all)g(of)
497271 > -150 3331 y(the)e(NPT)f(sim)n(ulations)f(w)n(ere)h(equilibrated)g(for)f
497272 > (100)g(ps)i(b)r(efore)-150 3426 y(a)36 b(200)f(ps)h(data)g(collection)g
497273 > (run,)i(and)f(they)f(used)g(the)h(previ-)-150 3522 y(ous)25
497274 > b(temp)r(erature's)g(\014nal)g(con\014guration)f(as)h(a)g(starting)f(p)
497275 > r(oin)n(t.)-150 3617 y(All)f(of)g(the)g(NVE)g(sim)n(ulations)f(had)h
497276 > (the)g(same)f(thermalization,)-150 3713 y(equilibration,)30
497277 > b(and)g(data)g(collection)f(times)h(stated)h(earlier)d(in)-150
497278 > 3808 y(this)g(pap)r(er.)-67 3903 y(Figure)i(9)g(sho)n(ws)g(the)h
497279 > (densit)n(y)g(pro\014le)f(for)g(the)h(SSD/E)g(w)n(a-)-150
497280 > 3999 y(ter)i(mo)r(del)h(in)f(comparison)f(to)h(the)h(original)e(SSD)i
497281 > (without)g(a)-150 4094 y(reaction)k(\014eld,)k(exp)r(erimen)n(t,)g(and)
497282 > d(the)g(other)g(common)g(w)n(a-)-150 4190 y(ter)f(mo)r(dels)g
497283 > (considered)f(previously)-7 b(.)68 b(The)38 b(calculated)g(den-)-150
497284 > 4285 y(sities)c(ha)n(v)n(e)e(increased)h(signi\014can)n(tly)g(o)n(v)n
497285 > (er)f(the)i(original)f(SSD)-150 4381 y(mo)r(del)28 b(and)h(matc)n(h)f
497286 > (the)g(exp)r(erimen)n(tal)g(v)-5 b(alue)28 b(just)h(b)r(elo)n(w)f(298)
497287 > -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
497288 > (is)f(0.995)p Ff(\006)p Fu(0.001)d(g/cm)1833 4446 y Fn(3)1869
497289 > 4476 y Fu(,)-150 4572 y(whic)n(h)k(compares)e(w)n(ell)h(with)i(the)f
497290 > (exp)r(erimen)n(tal)f(v)-5 b(alue)21 b(of)f(0.997)-150
497291 > 4667 y(g/cm)40 4637 y Fn(3)118 4667 y Fu(and)41 b(is)h(considerably)e
497292 > (b)r(etter)i(than)f(the)h(SSD)h(v)-5 b(alue)-150 4763
497293 > y(of)43 b(0.967)p Ff(\006)p Fu(0.003)38 b(g/cm)635 4733
497294 > y Fn(3)671 4763 y Fu(.)82 b(The)43 b(increased)f(dip)r(ole)g(momen)n(t)
497295 > -150 4858 y(in)33 b(SSD/E)f(has)f(help)r(ed)i(to)f(\015atten)h(out)f
497296 > (the)h(curv)n(e)e(at)h(higher)-150 4954 y(temp)r(eratures,)25
497297 > b(only)g(the)h(impro)n(v)n(emen)n(t)e(is)i(marginal)e(at)h(b)r(est.)
497298 > -150 5049 y(This)30 b(steep)f(drop)h(in)f(densities)h(is)g(due)g(to)f
497299 > (the)h(dip)r(olar)f(rather)-150 5145 y(than)24 b(c)n(harge)e(based)i
497300   (in)n(teractions)e(whic)n(h)i(deca)n(y)f(more)g(rapidly)-150
497301 < 4285 y(at)k(longer)g(distances.)-67 4381 y(By)35 b(monitoring)g(Cp)g
497302 < (throughout)g(these)g(sim)n(ulations,)i(the)-150 4476
497303 < y(melting)42 b(transition)f(for)g(SSD/E)g(w)n(as)g(observ)n(ed)f(at)h
497304 < (230)g(K,)-150 4572 y(ab)r(out)35 b(5)f(degrees)f(lo)n(w)n(er)g(than)i
497282 < (SSD.)g(The)g(resulting)f(densit)n(y)-150 4667 y(maxim)n(um)41
497283 < b(is)g(lo)r(cated)g(at)g(240)f(K,)h(again)f(ab)r(out)h(5)g(degrees)-150
497284 < 4763 y(lo)n(w)n(er)33 b(than)j(the)f(SSD)h(v)-5 b(alue)35
497285 < b(of)g(245)f(K.)g(Though)h(there)g(is)g(a)-150 4858 y(decrease)30
497286 < b(in)h(b)r(oth)h(of)f(these)h(v)-5 b(alues,)32 b(the)f(corrected)f
497287 < (densities)-150 4954 y(near)d(ro)r(om)f(temp)r(erature)i(justify)g(the)
497288 < g(mo)r(di\014cations)f(tak)n(en.)-67 5049 y(Figure)70
497289 < b(10)h(sho)n(ws)f(a)g(densit)n(y)h(comparison)e(b)r(et)n(w)n(een)-150
497290 < 5145 y(SSD/RF)41 b(and)f(SSD)i(with)f(an)f(activ)n(e)g(reaction)f
497291 < (\014eld.)76 b(Lik)n(e)-150 5240 y(in)35 b(the)g(sim)n(ulations)f(of)g
497292 < (SSD/E,)h(the)g(densities)g(sho)n(w)e(a)i(dra-)-150 5336
497293 < y(matic)26 b(increase)e(o)n(v)n(er)g(normal)h(SSD.)i(A)n(t)f(298)e(K,)i
497294 < (SSD/RF)g(has)2059 2245 y @beginspecial 44 @llx 93 @lly
497295 < 517 @urx 661 @ury 2409 @rwi @setspecial
497301 > 5240 y(at)k(longer)g(distances.)-67 5336 y(By)35 b(monitoring)g(Cp)g
497302 > (throughout)g(these)g(sim)n(ulations,)i(the)2059 2245
497303 > y @beginspecial 44 @llx 93 @lly 517 @urx 661 @ury 2409
497304 > @rwi @setspecial
497305   %%BeginDocument: ssdrfcompare.epsi
497306   %!PS-Adobe-2.0 EPSF-1.2
497307   %%Title: ssdrfcompare.ps
# Line 505848 | Line 505857 | cleartomark countdictstack exch sub { end } repeat res
505857   %%EOF
505858  
505859   %%EndDocument
505860 < @endspecial 2042 2415 a Fq(FIG.)d(10:)34 b(Comparison)23
505860 > @endspecial 2042 2415 a Fr(FIG.)23 b(10:)34 b(Comparison)23
505861   b(of)g(densities)h(calculated)f(with)g(SSD/RF)f(to)2042
505862   2502 y(SSD)i(with)i(a)g(reaction)g(\014eld,)g(TIP4P)3157
505863 < 2471 y Fc(18)3223 2502 y Fq(,)g(TIP3P)3495 2471 y Fc(18)3561
505864 < 2502 y Fq(,)g(SPC/E)3848 2471 y Fc(19)3914 2502 y Fq(,)f(and)2042
505865 < 2590 y(Exp)r(erimen)n(t)2435 2558 y Fc(20)2498 2590 y
505866 < Fq(.)55 b(The)32 b(upp)r(er)f(plot)i(includes)f(error)h(bars,)i(and)c
505863 > 2471 y Fc(19)3223 2502 y Fr(,)g(TIP3P)3495 2471 y Fc(19)3561
505864 > 2502 y Fr(,)g(SPC/E)3848 2471 y Fc(20)3914 2502 y Fr(,)f(and)2042
505865 > 2590 y(Exp)r(erimen)n(t)2435 2558 y Fc(21)2498 2590 y
505866 > Fr(.)55 b(The)32 b(upp)r(er)f(plot)i(includes)f(error)h(bars,)i(and)c
505867   (the)2042 2677 y(calculated)26 b(results)f(from)g(the)f(other)h
505868   (references)h(w)n(ere)g(remo)n(v)n(ed)d(for)2042 2764
505869 < y(clarit)n(y)-6 b(.)2042 3044 y Ft(a)37 b(densit)n(y)g(of)h(0.997)p
505870 < Fe(\006)p Ft(0.001)33 b(g/cm)3192 3014 y Fm(3)3229 3044
505871 < y Ft(,)40 b(righ)n(t)d(in)h(line)g(with)g(ex-)2042 3140
505869 > y(clarit)n(y)-6 b(.)2042 3044 y Fu(melting)42 b(transition)f(for)g
505870 > (SSD/E)g(w)n(as)g(observ)n(ed)f(at)h(230)f(K,)2042 3140
505871 > y(ab)r(out)34 b(5)g(degrees)g(lo)n(w)n(er)f(than)h(SSD.)i(The)e
505872 > (resulting)g(densit)n(y)2042 3235 y(maxim)n(um)41 b(is)g(lo)r(cated)g
505873 > (at)g(240)f(K,)h(again)f(ab)r(out)h(5)g(degrees)2042
505874 > 3331 y(lo)n(w)n(er)33 b(than)i(the)h(SSD)g(v)-5 b(alue)35
505875 > b(of)g(245)e(K.)i(Though)g(there)g(is)g(a)2042 3426 y(decrease)30
505876 > b(in)h(b)r(oth)h(of)f(these)h(v)-5 b(alues,)32 b(the)f(corrected)f
505877 > (densities)2042 3522 y(near)d(ro)r(om)f(temp)r(erature)h(justify)i(the)
505878 > f(mo)r(di\014cations)f(tak)n(en.)2125 3617 y(Figure)70
505879 > b(10)g(sho)n(ws)g(a)h(densit)n(y)g(comparison)e(b)r(et)n(w)n(een)2042
505880 > 3713 y(SSD/RF)41 b(and)f(SSD)h(with)g(an)g(activ)n(e)e(reaction)h
505881 > (\014eld.)76 b(Lik)n(e)2042 3808 y(in)35 b(the)g(sim)n(ulations)f(of)g
505882 > (SSD/E,)h(the)g(densities)f(sho)n(w)g(a)g(dra-)2042 3903
505883 > y(matic)26 b(increase)e(o)n(v)n(er)g(normal)h(SSD.)h(A)n(t)h(298)d(K,)h
505884 > (SSD/RF)i(has)2042 3999 y(a)37 b(densit)n(y)g(of)h(0.997)p
505885 > Ff(\006)p Fu(0.001)33 b(g/cm)3192 3969 y Fn(3)3229 3999
505886 > y Fu(,)40 b(righ)n(t)d(in)h(line)g(with)g(ex-)2042 4094
505887   y(p)r(erimen)n(t)28 b(and)g(considerably)e(b)r(etter)j(than)f(the)h
505888 < (SSD)f(v)-5 b(alue)28 b(of)2042 3235 y(0.941)p Fe(\006)p
505889 < Ft(0.001)34 b(g/cm)2713 3205 y Fm(3)2750 3235 y Ft(.)70
505888 > (SSD)f(v)-5 b(alue)28 b(of)2042 4190 y(0.941)p Ff(\006)p
505889 > Fu(0.001)34 b(g/cm)2713 4160 y Fn(3)2750 4190 y Fu(.)70
505890   b(The)38 b(melting)h(p)r(oin)n(t)g(is)f(observ)n(ed)f(at)2042
505891 < 3331 y(240)21 b(K,)i(whic)n(h)g(is)g(5)g(degrees)f(lo)n(w)n(er)f(than)i
505892 < (SSD)h(with)g(a)e(reaction)2042 3426 y(\014eld,)h(and)e(the)g(densit)n
505891 > 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
505892 > (SSD)h(with)g(a)e(reaction)2042 4381 y(\014eld,)h(and)e(the)g(densit)n
505893   (y)h(maxim)n(um)f(at)g(255)f(K,)h(again)f(5)h(degrees)2042
505894 < 3522 y(lo)n(w)n(er)26 b(than)j(SSD.)g(The)f(densit)n(y)g(at)g(higher)g
505895 < (temp)r(erature)g(still)2042 3617 y(drops)c(o\013)g(more)g(rapidly)g
505894 > 4476 y(lo)n(w)n(er)26 b(than)j(SSD.)g(The)f(densit)n(y)g(at)g(higher)g
505895 > (temp)r(erature)g(still)2042 4572 y(drops)c(o\013)g(more)g(rapidly)g
505896   (than)h(the)g(c)n(harge)e(based)h(mo)r(dels)h(but)2042
505897 < 3713 y(is)i(in)h(b)r(etter)g(agreemen)n(t)e(than)i(SSD/E.)2125
505898 < 3808 y(The)e(reparameterization)e(of)i(the)g(SSD)h(w)n(ater)e(mo)r
505899 < (del,)i(b)r(oth)2042 3903 y(for)34 b(use)g(with)h(and)g(without)f(an)h
505900 < (applied)f(long-range)e(correc-)2042 3999 y(tion,)41
505897 > 4667 y(is)i(in)h(b)r(etter)g(agreemen)n(t)e(than)i(SSD/E.)2125
505898 > 4763 y(The)e(reparameterization)e(of)i(the)g(SSD)h(w)n(ater)e(mo)r
505899 > (del,)i(b)r(oth)2042 4858 y(for)34 b(use)g(with)h(and)g(without)f(an)h
505900 > (applied)f(long-range)e(correc-)2042 4954 y(tion,)41
505901   b(brough)n(t)c(the)i(densities)f(up)h(to)f(what)g(is)g(exp)r(ected)h
505902 < (for)2042 4094 y(sim)n(ulating)f(liquid)i(w)n(ater.)70
505903 < b(In)40 b(addition)f(to)g(impro)n(ving)f(the)2042 4190
505902 > (for)2042 5049 y(sim)n(ulating)f(liquid)i(w)n(ater.)70
505903 > b(In)40 b(addition)f(to)g(impro)n(ving)f(the)2042 5145
505904   y(densities,)23 b(it)f(is)g(imp)r(ortan)n(t)f(that)h(particle)g(transp)
505905 < r(ort)e(b)r(e)j(main-)2042 4285 y(tained)f(or)f(impro)n(v)n(ed.)34
505905 > r(ort)e(b)r(e)j(main-)2042 5240 y(tained)f(or)f(impro)n(v)n(ed.)34
505906   b(Figure)22 b(11)f(compares)g(the)i(temp)r(erature)2042
505907 < 4381 y(dep)r(endence)35 b(of)g(the)g(di\013usion)g(constan)n(t)f(of)g
505908 < (SSD/E)h(to)f(SSD)2042 4476 y(without)41 b(an)f(activ)n(e)g(reaction)f
505885 < (\014eld,)44 b(b)r(oth)d(at)f(the)h(densities)2042 4572
505886 < y(calculated)24 b(at)g(1)g(atm)h(and)f(at)h(the)g(exp)r(erimen)n(tally)
505887 < f(calculated)2042 4667 y(densities)h(for)g(sup)r(er-co)r(oled)g(and)g
505888 < (liquid)h(w)n(ater.)35 b(In)26 b(the)g(upp)r(er)2042
505889 < 4763 y(plot,)35 b(the)f(di\013usion)g(constan)n(t)f(for)g(SSD/E)g(is)h
505890 < (consisten)n(tly)f(a)2042 4858 y(little)27 b(faster)g(than)g(exp)r
505891 < (erimen)n(t,)g(while)g(SSD)h(starts)e(o\013)h(slo)n(w)n(er)2042
505892 < 4954 y(than)39 b(exp)r(erimen)n(t)g(and)g(crosses)e(to)i(merge)f(with)i
505893 < (SSD/E)e(at)2042 5049 y(high)24 b(temp)r(eratures.)35
505894 < b(Both)24 b(mo)r(dels)g(follo)n(w)g(the)h(exp)r(erimen)n(tal)2042
505895 < 5145 y(trend)18 b(w)n(ell,)j(but)e(di\013use)g(to)r(o)f(rapidly)g(at)h
505896 < (higher)f(temp)r(eratures.)2042 5240 y(This)23 b(abnormally)f(fast)h
505897 < (di\013usion)h(is)f(caused)g(b)n(y)g(the)h(decreased)2042
505898 < 5336 y(system)h(densit)n(y)-7 b(.)37 b(Since)26 b(the)g(densities)g(of)
505899 < g(SSD/E)f(don't)i(devi-)p eop
505907 > 5336 y(dep)r(endence)35 b(of)g(the)g(di\013usion)g(constan)n(t)f(of)g
505908 > (SSD/E)h(to)f(SSD)p eop
505909   %%Page: 9 9
505910 < 9 8 bop 4043 -299 a Ft(9)-133 2393 y @beginspecial 63
505910 > 9 8 bop 4043 -299 a Fu(9)-133 2393 y @beginspecial 63
505911   @llx 92 @lly 515 @urx 668 @ury 2409 @rwi @setspecial
505912   %%BeginDocument: ssdediffuse.epsi
505913   %!PS-Adobe-2.0 EPSF-1.2
# Line 514393 | Line 514402 | cleartomark countdictstack exch sub { end } repeat res
514402   %%EOF
514403  
514404   %%EndDocument
514405 < @endspecial -150 2563 a Fq(FIG.)42 b(11:)66 b(Plots)42
514405 > @endspecial -150 2563 a Fr(FIG.)42 b(11:)66 b(Plots)42
514406   b(of)g(the)f(di\013usion)g(constan)n(ts)g(calculated)h(from)-150
514407   2650 y(SSD/E)36 b(and)g(SSD,)f(b)r(oth)h(without)h(a)f(reaction)i
514408   (\014eld)e(along)h(with)-150 2737 y(exp)r(erimen)n(tal)e(results)i
514409 < (from)f(Gillen)h Fr(et)h(al.)1184 2705 y Fc(21)1284 2737
514410 < y Fq(and)e(Mills)1607 2705 y Fc(22)1673 2737 y Fq(.)66
514409 > (from)f(Gillen)h Fs(et)h(al.)1184 2705 y Fc(22)1284 2737
514410 > y Fr(and)e(Mills)1607 2705 y Fc(23)1673 2737 y Fr(.)66
514411   b(The)-150 2824 y(upp)r(er)33 b(plot)h(is)g(at)g(densities)g
514412   (calculated)h(from)f(the)f(NPT)h(sim)n(ula-)-150 2912
514413   y(tions)f(at)h(a)f(pressure)g(of)h(1)f(atm,)h(while)g(the)f(lo)n(w)n
514414   (er)h(plot)f(is)h(at)f(the)-150 2999 y(exp)r(erimen)n(tally)25
514415 < b(calculated)h(densities.)-150 3279 y Ft(ate)i(as)f(m)n(uc)n(h)h(from)g
514416 < (exp)r(erimen)n(t)g(as)f(those)h(of)g(SSD,)h(it)f(follo)n(ws)-150
514417 < 3374 y(the)f(exp)r(erimen)n(tal)g(trend)g(more)f(closely)-7
514418 < b(.)36 b(This)27 b(observ)-5 b(ation)26 b(is)-150 3470
514419 < y(bac)n(k)n(ed)36 b(up)h(b)n(y)f(lo)r(oking)g(at)g(the)h(lo)n(w)n(er)e
514420 < (plot.)64 b(The)37 b(di\013usion)-150 3565 y(constan)n(ts)27
514421 < b(for)h(SSD/E)h(trac)n(k)e(with)i(the)g(exp)r(erimen)n(tal)f(v)-5
514422 < b(alues)-150 3661 y(while)28 b(SSD)g(deviates)g(on)f(the)h(lo)n(w)f
514423 < (side)h(of)f(the)i(trend)e(with)h(in-)-150 3756 y(creasing)d(temp)r
514415 > b(calculated)h(densities.)-150 3279 y Fu(without)41 b(an)f(activ)n(e)g
514416 > (reaction)f(\014eld,)44 b(b)r(oth)d(at)g(the)f(densities)-150
514417 > 3374 y(calculated)24 b(at)g(1)h(atm)f(and)h(at)f(the)h(exp)r(erimen)n
514418 > (tally)f(calculated)-150 3470 y(densities)i(for)f(sup)r(er-co)r(oled)f
514419 > (and)h(liquid)h(w)n(ater.)36 b(In)25 b(the)h(upp)r(er)-150
514420 > 3565 y(plot,)35 b(the)f(di\013usion)g(constan)n(t)f(for)g(SSD/E)g(is)h
514421 > (consisten)n(tly)f(a)-150 3661 y(little)28 b(faster)e(than)h(exp)r
514422 > (erimen)n(t,)g(while)g(SSD)h(starts)e(o\013)h(slo)n(w)n(er)-150
514423 > 3756 y(than)39 b(exp)r(erimen)n(t)g(and)g(crosses)e(to)i(merge)f(with)i
514424 > (SSD/E)f(at)-150 3852 y(high)24 b(temp)r(eratures.)35
514425 > b(Both)24 b(mo)r(dels)h(follo)n(w)e(the)i(exp)r(erimen)n(tal)-150
514426 > 3947 y(trend)19 b(w)n(ell,)h(but)f(di\013use)g(to)r(o)g(rapidly)f(at)g
514427 > (higher)g(temp)r(eratures.)-150 4043 y(This)23 b(abnormally)f(fast)h
514428 > (di\013usion)h(is)f(caused)g(b)n(y)g(the)h(decreased)-150
514429 > 4138 y(system)i(densit)n(y)-7 b(.)36 b(Since)26 b(the)g(densities)g(of)
514430 > g(SSD/E)g(don't)g(devi-)-150 4234 y(ate)i(as)f(m)n(uc)n(h)h(from)g(exp)
514431 > r(erimen)n(t)g(as)f(those)h(of)g(SSD,)h(it)f(follo)n(ws)-150
514432 > 4329 y(the)f(exp)r(erimen)n(tal)g(trend)g(more)f(closely)-7
514433 > b(.)36 b(This)27 b(observ)-5 b(ation)26 b(is)-150 4425
514434 > y(bac)n(k)n(ed)36 b(up)h(b)n(y)f(lo)r(oking)g(at)g(the)h(lo)n(w)n(er)e
514435 > (plot.)64 b(The)37 b(di\013usion)-150 4520 y(constan)n(ts)27
514436 > b(for)h(SSD/E)h(trac)n(k)e(with)i(the)g(exp)r(erimen)n(tal)f(v)-5
514437 > b(alues)-150 4616 y(while)28 b(SSD)g(deviates)g(on)f(the)h(lo)n(w)f
514438 > (side)h(of)f(the)i(trend)e(with)h(in-)-150 4711 y(creasing)d(temp)r
514439   (erature.)36 b(This)27 b(is)g(again)f(a)g(pro)r(duct)h(of)g(SSD/E)-150
514440 < 3852 y(ha)n(ving)g(densities)i(closer)e(to)h(exp)r(erimen)n(t,)h(and)f
514441 < (not)h(deviating)-150 3947 y(to)22 b(lo)n(w)n(er)e(densities)j(with)f
514440 > 4807 y(ha)n(ving)g(densities)i(closer)e(to)h(exp)r(erimen)n(t,)h(and)f
514441 > (not)h(deviating)-150 4902 y(to)22 b(lo)n(w)n(er)e(densities)j(with)f
514442   (increasing)f(temp)r(erature)h(as)f(rapidly)-7 b(.)-67
514443 < 4043 y(In)36 b(\014gure)f(12,)i(the)f(di\013usion)g(constan)n(ts)f(for)
514444 < g(SSD/RF)h(are)-150 4138 y(compared)k(with)j(SSD)f(with)g(an)g(activ)n
514445 < (e)e(reaction)h(\014eld.)79 b(In)-150 4234 y(the)39 b(upp)r(er)g(plot,)
514443 > 4997 y(In)36 b(\014gure)f(12,)i(the)f(di\013usion)g(constan)n(ts)f(for)
514444 > g(SSD/RF)h(are)-150 5093 y(compared)k(with)j(SSD)f(with)g(an)g(activ)n
514445 > (e)e(reaction)h(\014eld.)79 b(In)-150 5188 y(the)39 b(upp)r(er)g(plot,)
514446   j(SSD/RF)e(trac)n(ks)d(with)j(the)f(exp)r(erimen)n(tal)-150
514447 < 4329 y(results)27 b(incredibly)g(w)n(ell,)g(iden)n(tical)h(within)g
514448 < (error)d(throughout)-150 4425 y(the)f(temp)r(erature)f(range)g(and)g
514449 < (only)h(sho)n(wing)e(a)i(sligh)n(t)f(increas-)-150 4520
514450 < y(ing)g(trend)g(at)g(higher)g(temp)r(eratures.)34 b(SSD)24
514451 < b(also)e(trac)n(ks)g(exp)r(er-)-150 4616 y(imen)n(t)35
514428 < b(w)n(ell,)h(only)e(it)h(tends)g(to)f(di\013use)h(a)f(little)i(more)d
514429 < (slo)n(wly)-150 4711 y(at)f(lo)n(w)g(temp)r(eratures)g(and)g(deviates)g
514430 < (to)g(di\013use)h(to)r(o)f(rapidly)-150 4807 y(at)26
514431 < b(high)h(temp)r(eratures.)35 b(As)27 b(w)n(as)e(stated)i(in)f(the)h
514432 < (SSD/E)f(com-)-150 4902 y(parisons,)f(this)i(deviation)f(a)n(w)n(a)n(y)
514433 < f(from)h(the)i(ideal)e(trend)h(is)f(due)-150 4997 y(to)38
514434 < b(a)g(rapid)g(decrease)f(in)i(densit)n(y)f(at)g(higher)g(temp)r
514435 < (eratures.)-150 5093 y(SSD/RF)k(do)r(esn't)f(su\013er)h(from)f(this)g
514436 < (problem)g(as)g(m)n(uc)n(h)g(as)-150 5188 y(SSD,)36 b(b)r(ecause)f(the)
514437 < g(calculated)g(densities)g(are)f(more)g(true)i(to)-150
514438 < 5284 y(exp)r(erimen)n(t.)42 b(This)30 b(is)f(again)f(emphasized)h(in)h
514439 < (the)f(lo)n(w)n(er)f(plot,)-150 5379 y(where)d(SSD/RF)g(trac)n(ks)f
514440 < (the)h(exp)r(erimen)n(tal)g(di\013usion)g(exactly)2059
514441 < 2393 y @beginspecial 63 @llx 92 @lly 515 @urx 668 @ury
514442 < 2409 @rwi @setspecial
514447 > 5284 y(results)27 b(incredibly)g(w)n(ell,)g(iden)n(tical)h(within)g
514448 > (error)d(throughout)-150 5379 y(the)f(temp)r(erature)f(range)g(and)g
514449 > (only)h(sho)n(wing)e(a)i(sligh)n(t)f(increas-)2059 2393
514450 > y @beginspecial 63 @llx 92 @lly 515 @urx 668 @ury 2409
514451 > @rwi @setspecial
514452   %%BeginDocument: ssdrfdiffuse.epsi
514453   %!PS-Adobe-2.0 EPSF-1.2
514454   %%Title: ssdrfdiffuse.ps
# Line 522922 | Line 522931 | cleartomark countdictstack exch sub { end } repeat res
522931   %%EOF
522932  
522933   %%EndDocument
522934 < @endspecial 2042 2563 a Fq(FIG.)41 b(12:)66 b(Plots)43
522934 > @endspecial 2042 2563 a Fr(FIG.)41 b(12:)66 b(Plots)43
522935   b(of)f(the)e(di\013usion)i(constan)n(ts)f(calculated)h(from)2042
522936   2650 y(SSD/RF)31 b(and)i(SSD,)e(b)r(oth)i(with)g(an)f(activ)n(e)h
522937   (reaction)h(\014eld)e(along)2042 2737 y(with)38 b(exp)r(erimen)n(tal)e
522938 < (results)j(from)e(Gillen)i Fr(et)g(al.)3570 2705 y Fc(21)3672
522939 < 2737 y Fq(and)e(Mills)3996 2705 y Fc(22)4063 2737 y Fq(.)2042
522938 > (results)j(from)e(Gillen)i Fs(et)g(al.)3570 2705 y Fc(22)3672
522939 > 2737 y Fr(and)e(Mills)3996 2705 y Fc(23)4063 2737 y Fr(.)2042
522940   2824 y(The)27 b(upp)r(er)g(plot)g(is)h(at)f(densities)h(calculated)g
522941   (from)f(the)g(NPT)g(sim-)2042 2912 y(ulations)f(at)f(a)h(pressure)f(of)
522942   h(1)g(atm,)f(while)h(the)f(lo)n(w)n(er)h(plot)f(is)h(at)f(the)2042
522943   2999 y(exp)r(erimen)n(tally)g(calculated)h(densities.)2042
522944 < 3279 y Ft(while)20 b(SSD's)g(di\013usion)g(constan)n(ts)e(are)h(sligh)n
522945 < (tly)g(to)r(o)g(lo)n(w)g(due)h(to)2042 3374 y(its)26
522946 < b(need)g(for)f(a)h(lo)n(w)n(er)e(densit)n(y)i(at)g(the)g(sp)r
522947 < (eci\014ed)h(temp)r(erature.)2508 3651 y Fn(E.)88 b(Additional)32
522948 < b(Observ)-5 b(ations)2125 3864 y Ft(While)45 b(p)r(erforming)f(the)g
522949 < (melting)h(sequences)f(of)g(SSD/E,)2042 3960 y(some)29
522950 < b(in)n(teresting)g(observ)-5 b(ations)28 b(w)n(ere)h(made.)43
522951 < b(After)30 b(melting)2042 4055 y(at)k(230)f(K,)h(t)n(w)n(o)g(of)g(the)h
522952 < (systems)f(underw)n(en)n(t)g(crystallization)2042 4151
522953 < y(ev)n(en)n(ts)23 b(near)h(245)f(K.)h(As)g(the)h(heating)f(pro)r(cess)f
522954 < (con)n(tin)n(ued,)i(the)2042 4246 y(t)n(w)n(o)c(systems)g(remained)g
522955 < (crystalline)f(un)n(til)i(\014nally)f(melting)h(b)r(e-)2042
522956 < 4342 y(t)n(w)n(een)32 b(320)g(and)g(330)f(K.)i(These)f(sim)n(ulations)g
522957 < (w)n(ere)g(excluded)2042 4437 y(from)k(the)g(data)g(set)g(sho)n(wn)f
522958 < (in)h(\014gure)g(9)g(and)f(replaced)h(with)2042 4532
522959 < y(t)n(w)n(o)f(additional)g(melting)g(sequences)g(that)h(did)g(not)f
522960 < (undergo)2042 4628 y(this)j(anomalous)e(phase)h(transition,)i(while)f
522961 < (this)g(crystalliza-)2042 4723 y(tion)27 b(ev)n(en)n(t)h(w)n(as)e(in)n
522962 < (v)n(estigated)g(separately)-7 b(.)2125 4819 y(The)21
522963 < b(\014nal)g(con\014gurations)f(of)h(these)g(t)n(w)n(o)g(melting)g
522964 < (sequences)2042 4914 y(sho)n(ws)d(an)h(expanded)f(zeolite-lik)n(e)g
522965 < (crystal)h(structure)f(that)i(do)r(es)2042 5010 y(not)39
522966 < b(corresp)r(ond)e(to)i(an)n(y)f(kno)n(wn)h(form)f(of)h(ice.)71
522967 < b(F)-7 b(or)39 b(con)n(v)n(e-)2042 5105 y(nience)23 b(and)h(to)f(help)h
522968 < (distinguish)g(it)g(from)f(the)h(exp)r(erimen)n(tally)2042
522969 < 5201 y(observ)n(ed)32 b(forms)i(of)g(ice,)h(this)g(crystal)e(structure)
522970 < g(will)i(hence-)2042 5296 y(forth)29 b(b)r(e)h(referred)e(to)h(as)g
522971 < (ice-zero)f(\(ice)i(0\).)42 b(The)29 b(crystallinit)n(y)2042
522972 < 5392 y(w)n(as)d(extensiv)n(e)g(enough)g(than)h(a)f(near)g(ideal)h
522973 < (crystal)f(structure)p eop
522944 > 3279 y Fu(ing)d(trend)g(at)g(higher)f(temp)r(eratures.)35
522945 > b(SSD)24 b(also)e(trac)n(ks)g(exp)r(er-)2042 3374 y(imen)n(t)35
522946 > b(w)n(ell,)h(only)e(it)h(tends)g(to)f(di\013use)h(a)f(little)i(more)d
522947 > (slo)n(wly)2042 3470 y(at)f(lo)n(w)g(temp)r(eratures)g(and)g(deviates)g
522948 > (to)g(di\013use)h(to)r(o)f(rapidly)2042 3565 y(at)26
522949 > b(high)g(temp)r(eratures.)36 b(As)27 b(w)n(as)e(stated)h(in)h(the)g
522950 > (SSD/E)f(com-)2042 3661 y(parisons,)f(this)i(deviation)f(a)n(w)n(a)n(y)
522951 > f(from)h(the)h(ideal)g(trend)f(is)h(due)2042 3756 y(to)38
522952 > b(a)g(rapid)g(decrease)f(in)i(densit)n(y)f(at)g(higher)g(temp)r
522953 > (eratures.)2042 3852 y(SSD/RF)k(do)r(esn't)f(su\013er)g(from)g(this)h
522954 > (problem)f(as)g(m)n(uc)n(h)g(as)2042 3947 y(SSD,)36 b(b)r(ecause)e(the)
522955 > i(calculated)f(densities)g(are)f(more)g(true)h(to)2042
522956 > 4043 y(exp)r(erimen)n(t.)42 b(This)29 b(is)h(again)e(emphasized)h(in)g
522957 > (the)h(lo)n(w)n(er)e(plot,)2042 4138 y(where)c(SSD/RF)i(trac)n(ks)e
522958 > (the)h(exp)r(erimen)n(tal)g(di\013usion)g(exactly)2042
522959 > 4234 y(while)20 b(SSD's)g(di\013usion)g(constan)n(ts)e(are)h(sligh)n
522960 > (tly)g(to)r(o)g(lo)n(w)g(due)h(to)2042 4329 y(its)26
522961 > b(need)g(for)f(a)h(lo)n(w)n(er)e(densit)n(y)i(at)g(the)g(sp)r
522962 > (eci\014ed)h(temp)r(erature.)2508 4605 y Fo(E.)88 b(Additional)32
522963 > b(Observ)-5 b(ations)2125 4819 y Fu(While)45 b(p)r(erforming)f(the)g
522964 > (melting)h(sequences)f(of)g(SSD/E,)2042 4914 y(some)29
522965 > b(in)n(teresting)g(observ)-5 b(ations)28 b(w)n(ere)h(made.)43
522966 > b(After)30 b(melting)2042 5010 y(at)k(230)f(K,)h(t)n(w)n(o)g(of)g(the)h
522967 > (systems)f(underw)n(en)n(t)g(crystallization)2042 5105
522968 > y(ev)n(en)n(ts)23 b(near)h(245)f(K.)h(As)g(the)h(heating)f(pro)r(cess)f
522969 > (con)n(tin)n(ued,)i(the)2042 5201 y(t)n(w)n(o)c(systems)g(remained)g
522970 > (crystalline)f(un)n(til)i(\014nally)f(melting)h(b)r(e-)2042
522971 > 5296 y(t)n(w)n(een)32 b(320)g(and)g(330)f(K.)i(These)f(sim)n(ulations)g
522972 > (w)n(ere)g(excluded)2042 5392 y(from)k(the)g(data)g(set)g(sho)n(wn)f
522973 > (in)h(\014gure)g(9)g(and)f(replaced)h(with)p eop
522974   %%Page: 10 10
522975 < 10 9 bop 4001 -299 a Ft(10)-133 1529 y @beginspecial
522975 > 10 9 bop 4001 -299 a Fu(10)-133 1529 y @beginspecial
522976   0 @llx 0 @lly 1169 @urx 987 @ury 2409 @rwi @setspecial
522977   %%BeginDocument: povIce.ps
522978   %!PS-Adobe-3.0 EPSF-3.0
# Line 627906 | Line 627915 | showpage
627915   %%EOF
627916  
627917   %%EndDocument
627918 < @endspecial -150 1699 a Fq(FIG.)26 b(13:)35 b(Crystal)26
627918 > @endspecial -150 1699 a Fr(FIG.)26 b(13:)35 b(Crystal)26
627919   b(structure)e(of)i(an)g(ice)f(0)h(lattice)g(sho)n(wn)g(from)f(the)-150
627920 < 1787 y(\(001\))i(face.)103 3219 y @beginspecial 0 @llx
627921 < 0 @lly 232 @urx 196 @ury 1842 @rwi @setspecial
627920 > 1787 y(\(001\))i(face.)-150 2071 y Fu(t)n(w)n(o)35 b(additional)g
627921 > (melting)g(sequences)g(that)h(did)g(not)g(undergo)-150
627922 > 2166 y(this)i(anomalous)e(phase)h(transition,)j(while)d(this)h
627923 > (crystalliza-)-150 2262 y(tion)28 b(ev)n(en)n(t)f(w)n(as)f(in)n(v)n
627924 > (estigated)h(separately)-7 b(.)-67 2357 y(The)21 b(\014nal)g
627925 > (con\014gurations)f(of)h(these)g(t)n(w)n(o)g(melting)g(sequences)-150
627926 > 2453 y(sho)n(ws)d(an)h(expanded)g(zeolite-lik)n(e)f(crystal)g
627927 > (structure)g(that)i(do)r(es)-150 2548 y(not)39 b(corresp)r(ond)e(to)i
627928 > (an)n(y)g(kno)n(wn)f(form)h(of)g(ice.)71 b(F)-7 b(or)38
627929 > b(con)n(v)n(e-)-150 2644 y(nience)24 b(and)f(to)g(help)h(distinguish)g
627930 > (it)g(from)f(the)h(exp)r(erimen)n(tally)-150 2739 y(observ)n(ed)32
627931 > b(forms)i(of)g(ice,)i(this)e(crystal)f(structure)g(will)i(hence-)-150
627932 > 2835 y(forth)29 b(b)r(e)h(referred)e(to)i(as)e(ice-zero)g(\(ice)i(0\).)
627933 > 42 b(The)29 b(crystallinit)n(y)-150 2930 y(w)n(as)d(extensiv)n(e)g
627934 > (enough)g(than)h(a)g(near)f(ideal)g(crystal)g(structure)-150
627935 > 3026 y(could)31 b(b)r(e)h(obtained.)49 b(Figure)31 b(13)f(sho)n(ws)h
627936 > (the)h(rep)r(eating)f(crys-)-150 3121 y(tal)37 b(structure)f(of)h(a)g
627937 > (t)n(ypical)g(crystal)e(at)i(5)g(K.)g(The)g(unit)g(cell)-150
627938 > 3217 y(con)n(tains)28 b(eigh)n(t)g(molecules,)g(and)g(\014gure)g(14)g
627939 > (sho)n(ws)f(a)h(unit)h(cell)-150 3312 y(built)35 b(from)e(the)h(w)n
627940 > (ater)f(particle)h(cen)n(ter)f(of)h(masses)f(that)h(can)-150
627941 > 3408 y(b)r(e)i(used)f(to)g(construct)g(a)g(rep)r(eating)f(lattice,)j
627942 > (similar)e(to)g(\014g-)-150 3503 y(ure)28 b(13.)38 b(Eac)n(h)27
627943 > b(molecule)h(is)h(h)n(ydrogen)d(b)r(onded)j(to)f(four)g(other)-150
627944 > 3598 y(w)n(ater)c(molecules;)h(ho)n(w)n(ev)n(er,)e(the)i(h)n(ydrogen)e
627945 > (b)r(onds)i(are)e(\015exed)-150 3694 y(rather)31 b(than)h(p)r(erfectly)
627946 > g(straigh)n(t.)49 b(This)32 b(results)g(in)g(a)g(sk)n(ew)n(ed)-150
627947 > 3789 y(tetrahedral)c(geometry)g(ab)r(out)h(the)h(cen)n(tral)e
627948 > (molecule.)42 b(Lo)r(ok-)-150 3885 y(ing)36 b(bac)n(k)f(at)h(\014gure)g
627949 > (8,)i(it)e(is)h(easy)e(to)h(see)g(ho)n(w)f(these)h(\015exed)-150
627950 > 3980 y(h)n(ydrogen)20 b(b)r(onds)i(are)f(allo)n(w)n(ed)f(in)i(that)g
627951 > (the)g(attractiv)n(e)f(regions)-150 4076 y(are)30 b(conical)f(in)i
627952 > (shap)r(e,)g(with)g(the)g(greatest)f(attraction)f(in)i(the)-150
627953 > 4171 y(cen)n(tral)e(region.)44 b(Though)30 b(not)g(ideal,)h(these)g
627954 > (\015exed)f(h)n(ydrogen)-150 4267 y(b)r(onds)e(are)f(fa)n(v)n(orable)f
627955 > (enough)h(to)h(stabilize)g(an)g(en)n(tire)g(crystal)-150
627956 > 4362 y(generated)22 b(around)h(them.)36 b(In)24 b(fact,)h(the)f(imp)r
627957 > (erfect)g(ice)f(0)h(crys-)-150 4458 y(tals)e(w)n(ere)g(so)f(stable)h
627958 > (that)h(they)g(melted)g(at)f(greater)f(than)h(ro)r(om)-150
627959 > 4553 y(temp)r(erature.)-67 4649 y(The)29 b(initial)g(sim)n(ulations)e
627960 > (indicated)i(that)g(ice)f(0)h(is)f(the)h(pre-)-150 4744
627961 > y(ferred)37 b(ice)g(structure)f(for)h(at)g(least)g(SSD/E.)g(T)-7
627962 > b(o)37 b(v)n(erify)f(this,)-150 4840 y(a)h(comparison)f(w)n(as)g(made)i
627963 > (b)r(et)n(w)n(een)f(near)g(ideal)g(crystals)f(of)-150
627964 > 4935 y(ice)24 b Fj(I)7 4947 y Fi(h)50 4935 y Fu(,)h(ice)f
627965 > Fj(I)255 4947 y Fi(c)289 4935 y Fu(,)h(and)f(ice)f(0)h(at)g(constan)n
627966 > (t)f(pressure)f(with)j(SSD/E,)-150 5031 y(SSD/RF,)e(and)g(SSD.)g(Near)f
627967 > (ideal)h(v)n(ersions)d(of)j(the)g(three)f(t)n(yp)r(es)-150
627968 > 5126 y(of)32 b(crystals)f(w)n(ere)g(co)r(oled)g(to)64
627969 > b(1)31 b(K,)h(and)g(the)g(p)r(oten)n(tial)g(ener-)-150
627970 > 5222 y(gies)25 b(of)g(eac)n(h)g(w)n(ere)f(compared)h(using)g(all)g
627971 > (three)g(w)n(ater)f(mo)r(dels.)-150 5317 y(With)d(ev)n(ery)d(w)n(ater)h
627972 > (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-)
627973 > -150 5412 y(est)31 b(p)r(oten)n(tial)h(energy:)43 b(5\045)31
627974 > b(lo)n(w)n(er)f(than)h Fj(I)1239 5424 y Fi(h)1314 5412
627975 > y Fu(with)h(SSD,)g(6.5\045)2295 1131 y @beginspecial
627976 > 0 @llx 0 @lly 232 @urx 196 @ury 1842 @rwi @setspecial
627977   %%BeginDocument: ice0cell.eps
627978   %!PS-Adobe-3.1 EPSF-3.0
627979   %%Title: ice0cell.eps
# Line 635700 | Line 635764 | userdict /ai9_skip_data get exec
635764   %AI9_PrivateDataEnd
635765  
635766   %%EndDocument
635767 < @endspecial -150 3389 a(FIG.)h(14:)40 b(Simple)27 b(unit)g(cell)i(for)
635768 < f(constructing)g(ice)h(0.)41 b(In)27 b(this)h(cell,)-150
635769 < 3476 y Fp(c)e Fq(is)g(equal)g(to)g(0)p Fp(:)p Fq(4714)19
635770 < b Fa(\002)e Fp(a)p Fq(,)25 b(and)h(a)g(t)n(ypical)f(v)l(alue)h(for)g
635771 < Fp(a)g Fq(is)g(8.25)1764 3463 y(\027)1764 3476 y(A.)-150
635772 < 3756 y Ft(could)31 b(b)r(e)h(obtained.)49 b(Figure)31
635773 < b(13)f(sho)n(ws)h(the)h(rep)r(eating)f(crys-)-150 3852
635774 < y(tal)37 b(structure)f(of)h(a)g(t)n(ypical)g(crystal)e(at)i(5)g(K.)g
635775 < (The)g(unit)g(cell)-150 3947 y(con)n(tains)28 b(eigh)n(t)g(molecules,)g
635776 < (and)g(\014gure)g(14)g(sho)n(ws)f(a)h(unit)h(cell)-150
635777 < 4043 y(built)35 b(from)e(the)h(w)n(ater)f(particle)h(cen)n(ter)f(of)h
635778 < (masses)f(that)h(can)-150 4138 y(b)r(e)i(used)f(to)g(construct)g(a)g
635779 < (rep)r(eating)f(lattice,)j(similar)e(to)g(\014g-)-150
635780 < 4234 y(ure)28 b(13.)38 b(Eac)n(h)27 b(molecule)h(is)h(h)n(ydrogen)d(b)r
635781 < (onded)j(to)f(four)g(other)-150 4329 y(w)n(ater)c(molecules;)h(ho)n(w)n
635782 < (ev)n(er,)e(the)i(h)n(ydrogen)e(b)r(onds)i(are)e(\015exed)-150
635783 < 4425 y(rather)31 b(than)h(p)r(erfectly)g(straigh)n(t.)49
635784 < b(This)32 b(results)g(in)g(a)g(sk)n(ew)n(ed)-150 4520
635785 < y(tetrahedral)c(geometry)g(ab)r(out)h(the)h(cen)n(tral)e(molecule.)42
635786 < b(Lo)r(ok-)-150 4615 y(ing)36 b(bac)n(k)f(at)h(\014gure)g(8,)i(it)e(is)
635787 < h(easy)e(to)h(see)g(ho)n(w)f(these)h(\015exed)-150 4711
635788 < y(h)n(ydrogen)20 b(b)r(onds)i(are)f(allo)n(w)n(ed)f(in)i(that)g(the)g
635789 < (attractiv)n(e)f(regions)-150 4806 y(are)30 b(conical)f(in)i(shap)r(e,)
635790 < g(with)g(the)g(greatest)f(attraction)f(in)i(the)-150
635791 < 4902 y(cen)n(tral)e(region.)44 b(Though)30 b(not)g(ideal,)h(these)g
635792 < (\015exed)f(h)n(ydrogen)-150 4997 y(b)r(onds)e(are)f(fa)n(v)n(orable)f
635793 < (enough)h(to)h(stabilize)g(an)g(en)n(tire)g(crystal)-150
635794 < 5093 y(generated)22 b(around)h(them.)36 b(In)24 b(fact,)h(the)f(imp)r
635795 < (erfect)g(ice)f(0)h(crys-)-150 5188 y(tals)e(w)n(ere)g(so)f(stable)h
635796 < (that)h(they)g(melted)g(at)f(greater)f(than)h(ro)r(om)-150
635797 < 5284 y(temp)r(erature.)-67 5379 y(The)29 b(initial)g(sim)n(ulations)e
635734 < (indicated)i(that)g(ice)f(0)h(is)f(the)h(pre-)2042 -83
635735 < y(ferred)36 b(ice)h(structure)g(for)g(at)g(least)g(SSD/E.)g(T)-7
635736 < b(o)36 b(v)n(erify)h(this,)2042 12 y(a)g(comparison)f(w)n(as)g(made)i
635737 < (b)r(et)n(w)n(een)f(near)g(ideal)g(crystals)f(of)2042
635738 < 108 y(ice)24 b Fi(I)2199 120 y Fh(h)2242 108 y Ft(,)h(ice)f
635739 < Fi(I)2447 120 y Fh(c)2481 108 y Ft(,)h(and)e(ice)h(0)g(at)f(constan)n
635740 < (t)h(pressure)e(with)i(SSD/E,)2042 203 y(SSD/RF,)f(and)g(SSD.)g(Near)f
635741 < (ideal)g(v)n(ersions)f(of)i(the)g(three)f(t)n(yp)r(es)2042
635742 < 299 y(of)32 b(crystals)e(w)n(ere)h(co)r(oled)h(to)64
635743 < b(1)31 b(K,)h(and)g(the)g(p)r(oten)n(tial)g(ener-)2042
635744 < 394 y(gies)25 b(of)g(eac)n(h)g(w)n(ere)f(compared)g(using)h(all)h
635745 < (three)f(w)n(ater)f(mo)r(dels.)2042 490 y(With)c(ev)n(ery)f(w)n(ater)g
635746 < (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-)
635747 < 2042 585 y(est)31 b(p)r(oten)n(tial)g(energy:)44 b(5\045)31
635748 < b(lo)n(w)n(er)e(than)j Fi(I)3431 597 y Fh(h)3506 585
635749 < y Ft(with)g(SSD,)g(6.5\045)2042 681 y(lo)n(w)n(er)27
635750 < 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
635751 < (all)2042 776 y(three)35 b(of)g(these)h(w)n(ater)e(mo)r(dels,)k(ice)d
635752 < Fi(I)3302 788 y Fh(c)3372 776 y Ft(w)n(as)g(observ)n(ed)e(to)j(b)r(e)
635753 < 2042 872 y(2\045)23 b(less)g(stable)h(than)g(ice)f Fi(I)2908
635754 < 884 y Fh(h)2952 872 y Ft(.)36 b(In)23 b(addition)h(to)g(ha)n(ving)e
635755 < (the)i(lo)n(w-)2042 967 y(est)j(p)r(oten)n(tial)h(energy)-7
635756 < b(,)26 b(ice)i(0)f(w)n(as)g(the)h(most)f(expanded)g(of)h(the)2042
635757 < 1063 y(three)i(ice)h(crystals,)60 b(5\045)31 b(less)f(dense)g(than)h
635758 < (ice)g Fi(I)3633 1075 y Fh(h)3707 1063 y Ft(with)g(all)f(of)2042
635759 < 1158 y(the)h(w)n(ater)f(mo)r(dels.)47 b(In)31 b(all)g(three)g(w)n(ater)
635760 < f(mo)r(dels,)i(ice)f Fi(I)3887 1170 y Fh(c)3952 1158
635761 < y Ft(w)n(as)2042 1254 y(observ)n(ed)26 b(to)h(b)r(e)56
635762 < b(2\045)27 b(more)g(dense)h(than)f(ice)h Fi(I)3553 1266
635763 < y Fh(h)3596 1254 y Ft(.)2125 1349 y(In)c(addition)g(to)g(the)h(lo)n(w)e
635764 < (temp)r(erature)h(comparisons,)f(melt-)2042 1445 y(ing)38
635765 < b(sequences)g(w)n(ere)f(p)r(erformed)i(with)g(ice)f(0)g(as)g(the)h
635766 < (initial)2042 1540 y(con\014guration)19 b(using)h(SSD/E,)h(SSD/RF,)g
635767 < (and)g(SSD)g(b)r(oth)h(with)2042 1636 y(and)k(without)h(a)f(reaction)f
635768 < (\014eld.)36 b(The)27 b(melting)f(transitions)g(for)2042
635769 < 1731 y(b)r(oth)20 b(SSD/E)g(and)f(SSD)i(without)f(a)g(reaction)e
635770 < (\014eld)j(o)r(ccurred)d(at)2042 1826 y(temp)r(erature)29
635771 < b(in)g(excess)g(of)g(375)f(K.)h(SSD/RF)h(and)g(SSD)g(with)2042
635772 < 1922 y(a)c(reaction)f(\014eld)i(had)f(more)g(reasonable)e(melting)j
635773 < (transitions,)2042 2017 y(do)n(wn)h(near)f(325)g(K.)h(These)g(melting)h
635774 < (p)r(oin)n(t)g(observ)-5 b(ations)26 b(em-)2042 2113
635767 > @endspecial 2042 1301 a Fr(FIG.)c(14:)39 b(Simple)27
635768 > b(unit)h(cell)g(for)h(constructing)f(ice)h(0.)41 b(In)27
635769 > b(this)h(cell,)2042 1389 y Fq(c)e Fr(is)g(equal)g(to)f(0)p
635770 > Fq(:)p Fr(4714)20 b Fa(\002)d Fq(a)p Fr(,)25 b(and)h(a)g(t)n(ypical)f
635771 > (v)l(alue)h(for)g Fq(a)f Fr(is)i(8.25)3956 1376 y(\027)3956
635772 > 1389 y(A.)2042 1669 y Fu(lo)n(w)n(er)g(with)h(SSD/E,)h(and)f(7.5\045)f
635773 > (lo)n(w)n(er)g(with)i(SSD/RF.)g(In)f(all)2042 1764 y(three)35
635774 > b(of)g(these)h(w)n(ater)e(mo)r(dels,)k(ice)d Fj(I)3302
635775 > 1776 y Fi(c)3372 1764 y Fu(w)n(as)g(observ)n(ed)e(to)j(b)r(e)2042
635776 > 1860 y(2\045)23 b(less)g(stable)h(than)g(ice)f Fj(I)2908
635777 > 1872 y Fi(h)2952 1860 y Fu(.)36 b(In)23 b(addition)h(to)g(ha)n(ving)e
635778 > (the)i(lo)n(w-)2042 1955 y(est)j(p)r(oten)n(tial)h(energy)-7
635779 > b(,)26 b(ice)i(0)f(w)n(as)g(the)h(most)f(expanded)g(of)h(the)2042
635780 > 2051 y(three)i(ice)h(crystals,)60 b(5\045)31 b(less)f(dense)g(than)h
635781 > (ice)g Fj(I)3633 2063 y Fi(h)3707 2051 y Fu(with)g(all)f(of)2042
635782 > 2146 y(the)h(w)n(ater)f(mo)r(dels.)47 b(In)31 b(all)g(three)g(w)n(ater)
635783 > f(mo)r(dels,)i(ice)f Fj(I)3887 2158 y Fi(c)3952 2146
635784 > y Fu(w)n(as)2042 2242 y(observ)n(ed)26 b(to)h(b)r(e)56
635785 > b(2\045)27 b(more)g(dense)h(than)f(ice)h Fj(I)3553 2254
635786 > y Fi(h)3596 2242 y Fu(.)2125 2337 y(In)c(addition)g(to)g(the)h(lo)n(w)e
635787 > (temp)r(erature)h(comparisons,)f(melt-)2042 2433 y(ing)38
635788 > b(sequences)g(w)n(ere)f(p)r(erformed)i(with)g(ice)f(0)g(as)g(the)h
635789 > (initial)2042 2528 y(con\014guration)19 b(using)h(SSD/E,)h(SSD/RF,)g
635790 > (and)g(SSD)g(b)r(oth)h(with)2042 2624 y(and)k(without)h(a)f(reaction)f
635791 > (\014eld.)36 b(The)27 b(melting)f(transitions)g(for)2042
635792 > 2719 y(b)r(oth)20 b(SSD/E)g(and)f(SSD)i(without)f(a)g(reaction)e
635793 > (\014eld)j(o)r(ccurred)d(at)2042 2814 y(temp)r(erature)29
635794 > b(in)g(excess)g(of)g(375)f(K.)h(SSD/RF)h(and)g(SSD)g(with)2042
635795 > 2910 y(a)c(reaction)f(\014eld)i(had)f(more)g(reasonable)e(melting)j
635796 > (transitions,)2042 3005 y(do)n(wn)h(near)f(325)g(K.)h(These)g(melting)h
635797 > (p)r(oin)n(t)g(observ)-5 b(ations)26 b(em-)2042 3101
635798   y(phasize)34 b(ho)n(w)h(preferred)f(this)h(crystal)f(structure)h(is)g
635799 < (o)n(v)n(er)e(the)2042 2208 y(most)27 b(common)h(t)n(yp)r(es)f(of)h
635799 > (o)n(v)n(er)e(the)2042 3196 y(most)27 b(common)h(t)n(yp)r(es)f(of)h
635800   (ice)g(when)g(using)f(these)h(single)f(p)r(oin)n(t)2042
635801 < 2304 y(w)n(ater)f(mo)r(dels.)2125 2399 y(Recognizing)c(that)i(the)h(ab)
635801 > 3292 y(w)n(ater)f(mo)r(dels.)2125 3387 y(Recognizing)c(that)i(the)h(ab)
635802   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
635803 < 2495 y(the)32 b(most)f(stable)h(and)f(lo)n(w)n(est)g(densit)n(y)g
635804 < (crystal)g(structure)g(for)2042 2590 y(these)26 b(single)g(p)r(oin)n(t)
635803 > 3483 y(the)32 b(most)f(stable)h(and)f(lo)n(w)n(est)g(densit)n(y)g
635804 > (crystal)g(structure)g(for)2042 3578 y(these)26 b(single)g(p)r(oin)n(t)
635805   h(w)n(ater)f(mo)r(dels,)h(it)g(is)f(in)n(teresting)g(to)g(sp)r(ec-)2042
635806 < 2686 y(ulate)c(on)g(the)g(fa)n(v)n(orabilit)n(y)e(of)i(this)h(crystal)e
635807 < (structure)g(with)i(the)2042 2781 y(di\013eren)n(t)33
635806 > 3674 y(ulate)c(on)g(the)g(fa)n(v)n(orabilit)n(y)e(of)i(this)h(crystal)e
635807 > (structure)g(with)i(the)2042 3769 y(di\013eren)n(t)33
635808   b(c)n(harge)e(based)i(mo)r(dels.)53 b(As)33 b(a)f(quic)n(k)h(test,)i
635809 < (these)e(3)2042 2877 y(crystal)28 b(t)n(yp)r(es)h(w)n(ere)f(con)n(v)n
635809 > (these)e(3)2042 3865 y(crystal)28 b(t)n(yp)r(es)h(w)n(ere)f(con)n(v)n
635810   (erted)f(from)i(SSD)h(t)n(yp)r(e)f(particles)f(to)2042
635811 < 2972 y(TIP3P)h(w)n(aters)h(and)h(read)f(in)n(to)h(CHARMM.)3527
635812 < 2942 y Fm(29)3629 2972 y Ft(Iden)n(tical)f(en-)2042 3068
635811 > 3960 y(TIP3P)h(w)n(aters)h(and)h(read)f(in)n(to)h(CHARMM.)3527
635812 > 3930 y Fn(30)3629 3960 y Fu(Iden)n(tical)f(en-)2042 4056
635813   y(ergy)f(minimizations)i(w)n(ere)e(p)r(erformed)i(on)f(all)g(of)h
635814 < (these)f(crys-)2042 3163 y(tals)36 b(to)g(compare)e(the)j(system)f
635815 < (energies.)61 b(Again,)38 b(ice)e(0)f(w)n(as)2042 3259
635814 > (these)f(crys-)2042 4151 y(tals)36 b(to)g(compare)e(the)j(system)f
635815 > (energies.)61 b(Again,)38 b(ice)e(0)f(w)n(as)2042 4247
635816   y(observ)n(ed)23 b(to)i(ha)n(v)n(e)f(the)h(lo)n(w)n(est)f(total)h
635817 < (system)g(energy)-7 b(.)35 b(The)25 b(to-)2042 3354 y(tal)c(energy)e
635817 > (system)g(energy)-7 b(.)35 b(The)25 b(to-)2042 4342 y(tal)c(energy)e
635818   (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
635819 < Fi(I)3543 3366 y Fh(h)3586 3354 y Ft(,)h(whic)n(h)f(w)n(as)f(in)2042
635820 < 3450 y(turn)50 b(3\045)25 b(lo)n(w)n(er)e(than)i(ice)g
635821 < Fi(I)2948 3462 y Fh(c)2983 3450 y Ft(.)36 b(F)-7 b(rom)24
635822 < b(these)h(initial)h(results,)f(w)n(e)2042 3545 y(w)n(ould)g(not)h(b)r
635819 > Fj(I)3543 4354 y Fi(h)3586 4342 y Fu(,)h(whic)n(h)f(w)n(as)f(in)2042
635820 > 4438 y(turn)50 b(3\045)25 b(lo)n(w)n(er)e(than)i(ice)g
635821 > Fj(I)2948 4450 y Fi(c)2983 4438 y Fu(.)36 b(F)-7 b(rom)24
635822 > b(these)h(initial)h(results,)f(w)n(e)2042 4533 y(w)n(ould)g(not)h(b)r
635823   (e)g(surprised)e(if)i(results)f(from)h(the)g(other)f(common)2042
635824 < 3641 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
635825 < (lo)n(w)n(est)e(energy)g(crys-)2042 3736 y(tal)26 b(structure.)36
635824 > 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
635825 > (lo)n(w)n(est)e(energy)g(crys-)2042 4724 y(tal)26 b(structure.)36
635826   b(A)27 b(con)n(tin)n(uation)f(on)g(w)n(ork)f(studing)h(ice)h(0)f(with)
635827 < 2042 3831 y(m)n(ultip)r(oin)n(t)35 b(w)n(ater)f(mo)r(dels)h(will)g(b)r
635828 < (e)g(published)g(in)g(a)g(coming)2042 3927 y(article.)2631
635829 < 4203 y Fn(IV.)88 b(CONCLUSIONS)2125 4417 y Ft(The)49
635807 < b(densit)n(y)g(maxim)n(um)f(and)h(temp)r(erature)g(dep)r(enden)n(t)2042
635808 < 4512 y(transp)r(ort)25 b(for)h(the)g(SSD)h(w)n(ater)e(mo)r(del,)i(b)r
635809 < (oth)f(with)h(and)f(with-)2042 4608 y(out)j(the)g(use)g(of)g(reaction)e
635810 < (\014eld,)j(w)n(ere)e(studied)h(via)g(a)f(series)g(of)2042
635811 < 4703 y(NPT)h(and)g(NVE)g(sim)n(ulations.)41 b(The)29
635812 < b(constan)n(t)g(pressure)e(sim-)2042 4799 y(ulations)34
635813 < b(of)h(the)h(melting)f(of)g(b)r(oth)g Fi(I)3264 4811
635814 < y Fh(h)3343 4799 y Ft(and)g Fi(I)3548 4811 y Fh(c)3617
635815 < 4799 y Ft(ice)g(sho)n(w)n(ed)f(a)2042 4894 y(densit)n(y)c(maxim)n(um)f
635816 < (near)h(260)e(K.)i(In)g(most)g(cases,)g(the)g(calcu-)2042
635817 < 4990 y(lated)25 b(densities)f(w)n(ere)g(signi\014can)n(tly)g(lo)n(w)n
635818 < (er)f(than)i(the)g(densities)2042 5085 y(calculated)k(in)h(sim)n
635819 < (ulations)f(of)h(other)f(w)n(ater)g(mo)r(dels.)44 b(Analy-)2042
635820 < 5180 y(sis)24 b(of)g(particle)f(di\013usion)i(sho)n(w)n(ed)e(SSD)i(to)f
635821 < (capture)g(the)g(trans-)2042 5276 y(p)r(ort)d(prop)r(erties)f(of)i(exp)
635822 < r(erimen)n(tal)f(v)n(ery)f(w)n(ell)h(in)h(b)r(oth)g(the)f(nor-)2042
635823 < 5371 y(mal)27 b(and)h(sup)r(er-co)r(oled)e(liquid)i(regimes.)37
635824 < b(In)28 b(order)e(to)i(correct)p eop
635827 > 2042 4819 y(m)n(ultip)r(oin)n(t)35 b(w)n(ater)f(mo)r(dels)h(will)g(b)r
635828 > (e)g(published)g(in)g(a)g(coming)2042 4915 y(article.)p
635829 > eop
635830   %%Page: 11 11
635831 < 11 10 bop 4001 -299 a Ft(11)-150 -83 y(the)36 b(densit)n(y)f(b)r(eha)n
635832 < (vior,)h(SSD)f(w)n(as)g(reparameterized)e(for)i(use)-150
635833 < 12 y(b)r(oth)g(with)g(and)g(without)g(a)f(long-range)e(in)n(teraction)h
635834 < (correc-)-150 108 y(tion,)39 b(SSD/RF)e(and)f(SSD/E)h(resp)r(ectiv)n
635835 < (ely)-7 b(.)62 b(In)37 b(addition)g(to)-150 203 y(correcting)32
635836 < b(the)i(abnormally)e(lo)n(w)h(densities,)i(these)e(new)h(v)n(er-)-150
635837 < 299 y(sions)28 b(w)n(ere)f(sho)n(w)h(to)g(main)n(tain)g(or)g(impro)n(v)
635838 < n(e)f(up)r(on)i(the)f(trans-)-150 394 y(p)r(ort)f(and)f(structural)h
635839 < (features)f(of)h(the)g(original)e(w)n(ater)h(mo)r(del,)-150
635840 < 490 y(all)19 b(while)h(main)n(taining)e(the)i(fast)f(p)r(erformance)f
635841 < (of)i(the)f(SSD)i(w)n(a-)-150 585 y(ter)30 b(mo)r(del.)46
635842 < b(This)30 b(w)n(ork)f(sho)n(ws)g(these)i(simple)f(w)n(ater)f(mo)r
635843 < (dels,)-150 681 y(and)36 b(in)g(particular)f(SSD/E)g(and)h(SSD/RF,)h
635844 < (to)e(b)r(e)i(excellen)n(t)-150 776 y(c)n(hoices)31 b(to)g(represen)n
635845 < (t)g(explicit)h(w)n(ater)e(in)i(future)g(sim)n(ulations)-150
635846 < 872 y(of)c(bio)r(c)n(hemical)f(systems.)286 1148 y Fn(V.)87
635847 < b(A)n(CKNO)n(WLEDGMENTS)-67 1361 y Ft(The)29 b(authors)f(w)n(ould)g
635848 < (lik)n(e)g(to)h(thank)g(the)g(National)f(Science)-150
635849 < 1457 y(F)-7 b(oundation)21 b(for)f(funding)h(under)g(gran)n(t)e
635850 < (CHE-0134881.)31 b(Com-)-150 1552 y(putation)19 b(time)h(w)n(as)e(pro)n
635851 < (vided)g(b)n(y)g(the)i(Notre)e(Dame)h(Bunc)n(h-of-)-150
635852 < 1648 y(Bo)n(xes)29 b(\(B.o.B\))i(computer)g(cluster)f(under)h(NSF)g
635853 < (gran)n(t)f(DMR)-150 1743 y(00)d(79647.)570 2020 y Fn(REFERENCES)-117
635854 < 2203 y Fm(1)-46 2233 y Ft(W.)39 b(L.)g(Jorgensen,)h(J.)f
635855 < (Chandrasekhar,)h(J.)f(D.)g(Madura,)-46 2329 y(R.)c(W.)h(Imp)r(ey)-7
635856 < b(,)38 b(and)d(M.)g(L.)h(Klein,)h(J.)e(Chem.)g(Ph)n(ys.)g
635857 < Fg(79)p Ft(,)-46 2424 y(926)26 b(\(1983\).)-117 2489
635858 < y Fm(2)-46 2520 y Ft(H.)62 b(J.)f(C.)h(Berendsen,)69
635831 > 11 10 bop 4001 -299 a Fu(11)439 -83 y Fo(IV.)88 b(CONCLUSIONS)-67
635832 > 131 y Fu(The)49 b(densit)n(y)g(maxim)n(um)f(and)h(temp)r(erature)g(dep)
635833 > r(enden)n(t)-150 226 y(transp)r(ort)25 b(for)h(the)g(SSD)h(w)n(ater)e
635834 > (mo)r(del,)i(b)r(oth)g(with)f(and)g(with-)-150 322 y(out)j(the)g(use)g
635835 > (of)g(reaction)f(\014eld,)h(w)n(ere)f(studied)i(via)e(a)h(series)e(of)
635836 > -150 417 y(NPT)i(and)g(NVE)g(sim)n(ulations.)41 b(The)29
635837 > b(constan)n(t)g(pressure)f(sim-)-150 512 y(ulations)34
635838 > b(of)h(the)h(melting)f(of)g(b)r(oth)g Fj(I)1072 524 y
635839 > Fi(h)1151 512 y Fu(and)g Fj(I)1356 524 y Fi(c)1425 512
635840 > y Fu(ice)g(sho)n(w)n(ed)f(a)-150 608 y(densit)n(y)c(maxim)n(um)g(near)f
635841 > (260)f(K.)i(In)g(most)g(cases,)g(the)g(calcu-)-150 703
635842 > y(lated)25 b(densities)g(w)n(ere)e(signi\014can)n(tly)h(lo)n(w)n(er)f
635843 > (than)i(the)g(densities)-150 799 y(calculated)k(in)h(sim)n(ulations)f
635844 > (of)h(other)g(w)n(ater)e(mo)r(dels.)44 b(Analy-)-150
635845 > 894 y(sis)24 b(of)g(particle)g(di\013usion)g(sho)n(w)n(ed)f(SSD)i(to)f
635846 > (capture)g(the)g(trans-)-150 990 y(p)r(ort)d(prop)r(erties)g(of)g(exp)r
635847 > (erimen)n(tal)g(v)n(ery)f(w)n(ell)h(in)h(b)r(oth)g(the)g(nor-)-150
635848 > 1085 y(mal)28 b(and)f(sup)r(er-co)r(oled)g(liquid)h(regimes.)36
635849 > b(In)28 b(order)e(to)i(correct)-150 1181 y(the)36 b(densit)n(y)f(b)r
635850 > (eha)n(vior,)h(SSD)f(w)n(as)g(reparameterized)e(for)i(use)-150
635851 > 1276 y(b)r(oth)g(with)g(and)g(without)g(a)f(long-range)e(in)n
635852 > (teraction)h(correc-)-150 1372 y(tion,)39 b(SSD/RF)e(and)f(SSD/E)h
635853 > (resp)r(ectiv)n(ely)-7 b(.)62 b(In)37 b(addition)g(to)-150
635854 > 1467 y(correcting)32 b(the)i(abnormally)e(lo)n(w)h(densities,)i(these)e
635855 > (new)h(v)n(er-)-150 1563 y(sions)28 b(w)n(ere)f(sho)n(w)h(to)g(main)n
635856 > (tain)g(or)g(impro)n(v)n(e)f(up)r(on)i(the)f(trans-)-150
635857 > 1658 y(p)r(ort)f(and)f(structural)h(features)f(of)h(the)g(original)e(w)
635858 > n(ater)h(mo)r(del,)-150 1754 y(all)19 b(while)h(main)n(taining)e(the)i
635859 > (fast)f(p)r(erformance)f(of)i(the)f(SSD)i(w)n(a-)-150
635860 > 1849 y(ter)30 b(mo)r(del.)46 b(This)30 b(w)n(ork)f(sho)n(ws)g(these)i
635861 > (simple)f(w)n(ater)f(mo)r(dels,)-150 1945 y(and)36 b(in)g(particular)f
635862 > (SSD/E)g(and)h(SSD/RF,)h(to)e(b)r(e)i(excellen)n(t)-150
635863 > 2040 y(c)n(hoices)31 b(to)g(represen)n(t)g(explicit)h(w)n(ater)e(in)i
635864 > (future)g(sim)n(ulations)-150 2136 y(of)c(bio)r(c)n(hemical)f(systems.)
635865 > 286 2412 y Fo(V.)87 b(A)n(CKNO)n(WLEDGMENTS)-67 2625
635866 > y Fu(The)29 b(authors)f(w)n(ould)g(lik)n(e)g(to)h(thank)g(the)g
635867 > (National)f(Science)-150 2721 y(F)-7 b(oundation)21 b(for)f(funding)h
635868 > (under)g(gran)n(t)e(CHE-0134881.)31 b(Com-)-150 2816
635869 > y(putation)19 b(time)h(w)n(as)e(pro)n(vided)g(b)n(y)g(the)i(Notre)e
635870 > (Dame)h(Bunc)n(h-of-)-150 2912 y(Bo)n(xes)29 b(\(B.o.B\))i(computer)g
635871 > (cluster)f(under)h(NSF)g(gran)n(t)f(DMR)-150 3007 y(00)d(79647.)570
635872 > 3283 y Fo(REFERENCES)-117 3467 y Fn(1)-46 3497 y Fu(W.)39
635873 > b(L.)g(Jorgensen,)h(J.)f(Chandrasekhar,)h(J.)f(D.)g(Madura,)-46
635874 > 3592 y(R.)c(W.)h(Imp)r(ey)-7 b(,)38 b(and)d(M.)g(L.)h(Klein,)h(J.)e
635875 > (Chem.)g(Ph)n(ys.)g Fh(79)p Fu(,)-46 3688 y(926)26 b(\(1983\).)-117
635876 > 3753 y Fn(2)-46 3783 y Fu(H.)62 b(J.)f(C.)h(Berendsen,)69
635877   b(J.)62 b(R.)g(Grigera,)68 b(and)62 b(T.)g(P)-7 b(.)-46
635878 < 2615 y(Straatsma,)26 b(J.)h(Ph)n(ys.)g(Chem.)h Fg(91)p
635879 < Ft(,)f(6269)f(\(1987\).)-117 2680 y Fm(3)-46 2710 y Ft(M.)c(W.)h
635878 > 3879 y(Straatsma,)26 b(J.)h(Ph)n(ys.)g(Chem.)h Fh(91)p
635879 > Fu(,)f(6269)f(\(1987\).)-117 3944 y Fn(3)-46 3974 y Fu(M.)c(W.)h
635880   (Mahoney)e(and)h(W.)g(L.)h(Jorgensen,)e(J.)h(Chem.)g(Ph)n(ys.)-46
635881 < 2806 y Fg(112)p Ft(\(20\),)k(8910)g(\(2000\).)-117 2871
635882 < y Fm(4)-46 2901 y Ft(M.)c(W.)h(Mahoney)e(and)h(W.)g(L.)h(Jorgensen,)e
635883 < (J.)h(Chem.)g(Ph)n(ys.)-46 2997 y Fg(114)p Ft(\(1\),)27
635884 < b(363)f(\(2001\).)-117 3062 y Fm(5)-46 3092 y Ft(Y.)19
635881 > 4070 y Fh(112)p Fu(\(20\),)k(8910)g(\(2000\).)-117 4135
635882 > y Fn(4)-46 4165 y Fu(M.)c(W.)h(Mahoney)e(and)h(W.)g(L.)h(Jorgensen,)e
635883 > (J.)h(Chem.)g(Ph)n(ys.)-46 4261 y Fh(114)p Fu(\(1\),)27
635884 > b(363)f(\(2001\).)-117 4326 y Fn(5)-46 4356 y Fu(Y.)19
635885   b(Liu)g(and)g(T.)g(Ic)n(hiy)n(e,)h(J.)e(Ph)n(ys.)g(Chem.)i
635886 < Fg(100)p Ft(,)g(2723)d(\(1996\).)-117 3158 y Fm(6)-46
635887 < 3188 y Ft(D.)36 b(Bratk)n(o,)h(L.)f(Blum,)j(and)d(A.)h(Luzar,)h(J.)e
635888 < (Chem.)g(Ph)n(ys.)-46 3283 y Fg(83)p Ft(\(12\),)26 b(6367)g(\(1985\).)
635889 < -117 3349 y Fm(7)-46 3379 y Ft(L.)32 b(Blum,)h(F.)f(V)-7
635890 < b(ericat,)33 b(and)f(D.)h(Bratk)n(o,)e(J.)h(Chem.)g(Ph)n(ys.)-46
635891 < 3474 y Fg(102)p Ft(\(3\),)27 b(1461)e(\(1995\).)-117
635892 < 3540 y Fm(8)-46 3570 y Ft(A.)39 b(Chandra)f(and)g(T.)h(Ic)n(hiy)n(e,)i
635893 < (J.)e(Chem.)g(Ph)n(ys.)f Fg(111)p Ft(\(6\),)-46 3665
635894 < y(2701)25 b(\(1999\).)-117 3731 y Fm(9)-46 3761 y Ft(Y.)41
635895 < b(Liu)g(and)g(T.)h(Ic)n(hiy)n(e,)i(Chem.)d(Ph)n(ys.)f(Lett.)i
635896 < Fg(256)p Ft(,)i(334)-46 3856 y(\(1996\).)2042 -113 y
635897 < Fm(10)2145 -83 y Ft(M.)25 b(P)-7 b(.)24 b(Allen)h(and)g(D.)g(J.)f
635898 < (Tildesley)-7 b(,)25 b Fl(Computer)j(Simulation)2145
635899 < 12 y(of)d(Liquids)k Ft(\(Oxford)20 b(Univ)n(ersit)n(y)g(Press,)h(New)g
635900 < (Y)-7 b(ork,)22 b(1987\).)2042 78 y Fm(11)2145 108 y
635901 < Ft(D.)42 b(v)-5 b(an)41 b(der)f(Sp)r(o)r(el,)45 b(P)-7
635902 < b(.)41 b(J.)f(v)-5 b(an)41 b(Maaren,)i(and)e(H.)g(J.)g(C.)2145
635903 < 203 y(Berendsen,)27 b(J.)h(Chem.)g(Ph)n(ys.)e Fg(111)p
635904 < Ft(\(6\),)h(10220)e(\(1998\).)2042 269 y Fm(12)2145 299
635905 < y Ft(W.)j(G.)g(Ho)r(o)n(v)n(er,)e(Ph)n(ys.)h(Rev.)g(A)h
635906 < Fg(31)p Ft(\(3\),)g(1695)d(\(1985\).)2042 364 y Fm(13)2145
635907 < 394 y Ft(W.)j(G.)g(Ho)r(o)n(v)n(er,)e(Ph)n(ys.)h(Rev.)g(A)h
635908 < Fg(34)p Ft(\(3\),)g(2499)d(\(1986\).)2042 460 y Fm(14)2145
635909 < 490 y Ft(A.)35 b(Dullw)n(eb)r(er,)h(B.)d(Leimkuhler,)j(and)e(R.)g
635910 < (McLac)n(hlan,)g(J.)2145 585 y(Chem.)28 b(Ph)n(ys.)f
635911 < Fg(107)p Ft(\(15\),)f(5840)g(\(1997\).)2042 651 y Fm(15)2145
635912 < 681 y Ft(A.)31 b(Kol,)f(B.)g(B.)g(Laird,)g(and)g(B.)g(J.)g(Leimkuhler,)
635913 < h(J.)f(Chem.)2145 776 y(Ph)n(ys.)d Fg(107)p Ft(\(7\),)g(2580)f
635914 < (\(1997\).)2042 842 y Fm(16)2145 872 y Ft(J.)g(D.)g(Bernal)f(and)h(R.)g
635915 < (H.)g(F)-7 b(o)n(wler,)26 b(J.)f(Chem.)i(Ph)n(ys.)d Fg(1)p
635916 < Ft(,)j(515)2145 967 y(\(1933\).)2042 1033 y Fm(17)2145
635917 < 1063 y Ft(A.)20 b(Rahman)f(and)g(F.)g(H.)h(Stillinger,)h(J.)e(Chem.)g
635918 < (Ph)n(ys.)g Fg(57)p Ft(\(9\),)2145 1158 y(4009)26 b(\(1972\).)2042
635919 < 1224 y Fm(18)2145 1254 y Ft(W.)37 b(L.)f(Jorgensen)f(and)h(C.)g
635920 < (Jenson,)i(J.)e(Comput.)h(Chem.)2145 1349 y Fg(19)p Ft(\(10\),)27
635921 < b(1179)f(\(1998\).)2042 1414 y Fm(19)2145 1445 y Ft(L.)35
635922 < b(A.)g(B\023)-42 b(aez)34 b(and)h(P)-7 b(.)35 b(Clancy)-7
635923 < b(,)36 b(J.)e(Chem.)h(Ph)n(ys.)f Fg(101)p Ft(\(11\),)2145
635924 < 1540 y(9837)26 b(\(1994\).)2042 1605 y Fm(20)2145 1636
635925 < y Ft(R.)37 b(C.)g(W)-7 b(east,)39 b(ed.,)h Fl(CR)n(C)e(Handb)l(o)l(ok)h
635926 < (of)g(Chemistry)h(and)2145 1731 y(Physics)50 b Ft(\(CR)n(C)41
635927 < b(Press,)j(Inc.,)h(Bo)r(ca)40 b(Raton,)k(FL,)e(1980\),)2145
635928 < 1826 y(60th)27 b(ed.)2042 1892 y Fm(21)2145 1922 y Ft(Gillen,)33
635929 < b(Douglas,)f(and)f(Ho)r(c)n(h,)h(J.)g(Chem.)g(Ph)n(ys.)e
635930 < Fg(57)p Ft(,)i(5117)2145 2017 y(\(1972\).)2042 2083 y
635931 < Fm(22)2145 2113 y Ft(R.)c(Mills,)g(J.)f(Ph)n(ys.)g(Chem.)h
635932 < Fg(77)p Ft(\(5\),)f(685)f(\(1973\).)2042 2178 y Fm(23)2145
635933 < 2208 y Ft(G.)d(Hura,)g(J.)f(M.)h(Sorenson,)f(R.)g(M.)h(Glaeser,)f(and)g
635934 < (T.)h(Head-)2145 2304 y(Gordon,)k(J.)g(Chem.)h(Ph)n(ys.)f
635935 < Fg(113)p Ft(\(20\),)f(9140)g(\(2000\).)2042 2369 y Fm(24)2145
635936 < 2399 y Ft(A.)h(K.)e(Sop)r(er)h(and)g(M.)g(G.)g(Phillips,)g(Chem.)h(Ph)n
635937 < (ys.)e Fg(107)p Ft(\(1\),)2145 2495 y(47)i(\(1986\).)2042
635938 < 2560 y Fm(25)2145 2590 y Ft(M.)h(Sprik,)g(J.)f(Chem.)h(Ph)n(ys.)e
635939 < Fg(95)p Ft(\(9\),)i(6762)d(\(1991\).)2042 2656 y Fm(26)2145
635940 < 2686 y Ft(A.)36 b(V.)g(Gubsk)-5 b(a)n(y)n(a)35 b(and)g(P)-7
635941 < b(.)35 b(G.)h(Kusalik,)h(J.)e(Chem.)h(Ph)n(ys.)2145 2781
635942 < y Fg(117)p Ft(\(11\),)27 b(5290)f(\(2002\).)2042 2847
635943 < y Fm(27)2145 2877 y Ft(Y.)e(S.)f(Bady)n(al,)g(M.)g(L.)g(Sab)r(oungi,)g
635944 < (D.)h(L.)f(Price,)g(S.)g(D.)h(Shas-)2145 2972 y(tri,)30
635886 > Fh(100)p Fu(,)g(2723)d(\(1996\).)-117 4422 y Fn(6)-46
635887 > 4452 y Fu(D.)36 b(Bratk)n(o,)h(L.)f(Blum,)j(and)d(A.)h(Luzar,)h(J.)e
635888 > (Chem.)g(Ph)n(ys.)-46 4547 y Fh(83)p Fu(\(12\),)26 b(6367)g(\(1985\).)
635889 > 2075 -113 y Fn(7)2145 -83 y Fu(L.)32 b(Blum,)i(F.)e(V)-7
635890 > b(ericat,)33 b(and)f(D.)h(Bratk)n(o,)e(J.)h(Chem.)g(Ph)n(ys.)2145
635891 > 12 y Fh(102)p Fu(\(3\),)27 b(1461)f(\(1995\).)2075 78
635892 > y Fn(8)2145 108 y Fu(A.)40 b(Chandra)d(and)i(T.)g(Ic)n(hiy)n(e,)i(J.)e
635893 > (Chem.)g(Ph)n(ys.)f Fh(111)p Fu(\(6\),)2145 203 y(2701)26
635894 > b(\(1999\).)2075 269 y Fn(9)2145 299 y Fu(C.)46 b(Sagui)e(and)h(T.)g
635895 > (A.)h(Darden,)j(Ann)n(u.)d(Rev.)f(Bioph)n(ys.)2145 394
635896 > y(Biomol.)27 b(Struct.)h Fh(28)p Fu(,)f(155)g(\(1999\).)2042
635897 > 460 y Fn(10)2145 490 y Fu(Y.)42 b(Liu)f(and)g(T.)g(Ic)n(hiy)n(e,)j
635898 > (Chem.)e(Ph)n(ys.)e(Lett.)i Fh(256)p Fu(,)i(334)2145
635899 > 585 y(\(1996\).)2042 651 y Fn(11)2145 681 y Fu(M.)25
635900 > b(P)-7 b(.)24 b(Allen)h(and)g(D.)g(J.)f(Tildesley)-7
635901 > b(,)25 b Fm(Computer)j(Simulation)2145 776 y(of)d(Liquids)k
635902 > Fu(\(Oxford)20 b(Univ)n(ersit)n(y)g(Press,)h(New)g(Y)-7
635903 > b(ork,)22 b(1987\).)2042 842 y Fn(12)2145 872 y Fu(D.)42
635904 > b(v)-5 b(an)41 b(der)f(Sp)r(o)r(el,)45 b(P)-7 b(.)41
635905 > b(J.)f(v)-5 b(an)41 b(Maaren,)i(and)e(H.)g(J.)g(C.)2145
635906 > 967 y(Berendsen,)27 b(J.)h(Chem.)g(Ph)n(ys.)e Fh(111)p
635907 > Fu(\(6\),)h(10220)e(\(1998\).)2042 1033 y Fn(13)2145
635908 > 1063 y Fu(W.)j(G.)g(Ho)r(o)n(v)n(er,)e(Ph)n(ys.)h(Rev.)g(A)h
635909 > Fh(31)p Fu(\(3\),)g(1695)d(\(1985\).)2042 1128 y Fn(14)2145
635910 > 1158 y Fu(W.)j(G.)g(Ho)r(o)n(v)n(er,)e(Ph)n(ys.)h(Rev.)g(A)h
635911 > Fh(34)p Fu(\(3\),)g(2499)d(\(1986\).)2042 1224 y Fn(15)2145
635912 > 1254 y Fu(A.)35 b(Dullw)n(eb)r(er,)h(B.)d(Leimkuhler,)j(and)e(R.)g
635913 > (McLac)n(hlan,)g(J.)2145 1349 y(Chem.)28 b(Ph)n(ys.)f
635914 > Fh(107)p Fu(\(15\),)f(5840)g(\(1997\).)2042 1414 y Fn(16)2145
635915 > 1445 y Fu(A.)31 b(Kol,)f(B.)g(B.)g(Laird,)g(and)g(B.)g(J.)g
635916 > (Leimkuhler,)h(J.)f(Chem.)2145 1540 y(Ph)n(ys.)d Fh(107)p
635917 > Fu(\(7\),)g(2580)f(\(1997\).)2042 1605 y Fn(17)2145 1636
635918 > y Fu(J.)g(D.)g(Bernal)f(and)h(R.)g(H.)g(F)-7 b(o)n(wler,)26
635919 > b(J.)f(Chem.)i(Ph)n(ys.)d Fh(1)p Fu(,)j(515)2145 1731
635920 > y(\(1933\).)2042 1796 y Fn(18)2145 1826 y Fu(A.)20 b(Rahman)f(and)g(F.)
635921 > g(H.)h(Stillinger,)h(J.)e(Chem.)g(Ph)n(ys.)g Fh(57)p
635922 > Fu(\(9\),)2145 1922 y(4009)26 b(\(1972\).)2042 1987 y
635923 > Fn(19)2145 2017 y Fu(W.)37 b(L.)f(Jorgensen)f(and)h(C.)g(Jenson,)i(J.)e
635924 > (Comput.)h(Chem.)2145 2113 y Fh(19)p Fu(\(10\),)27 b(1179)f(\(1998\).)
635925 > 2042 2178 y Fn(20)2145 2208 y Fu(L.)35 b(A.)g(B\023)-42
635926 > b(aez)34 b(and)h(P)-7 b(.)35 b(Clancy)-7 b(,)36 b(J.)e(Chem.)h(Ph)n
635927 > (ys.)f Fh(101)p Fu(\(11\),)2145 2304 y(9837)26 b(\(1994\).)2042
635928 > 2369 y Fn(21)2145 2399 y Fu(R.)37 b(C.)g(W)-7 b(east,)39
635929 > b(ed.,)h Fm(CR)n(C)e(Handb)l(o)l(ok)h(of)g(Chemistry)h(and)2145
635930 > 2495 y(Physics)50 b Fu(\(CR)n(C)41 b(Press,)j(Inc.,)h(Bo)r(ca)40
635931 > b(Raton,)k(FL,)e(1980\),)2145 2590 y(60th)27 b(ed.)2042
635932 > 2656 y Fn(22)2145 2686 y Fu(Gillen,)33 b(Douglas,)f(and)f(Ho)r(c)n(h,)h
635933 > (J.)g(Chem.)g(Ph)n(ys.)e Fh(57)p Fu(,)i(5117)2145 2781
635934 > y(\(1972\).)2042 2847 y Fn(23)2145 2877 y Fu(R.)c(Mills,)g(J.)f(Ph)n
635935 > (ys.)g(Chem.)h Fh(77)p Fu(\(5\),)f(685)f(\(1973\).)2042
635936 > 2942 y Fn(24)2145 2972 y Fu(G.)d(Hura,)g(J.)f(M.)h(Sorenson,)f(R.)g(M.)
635937 > h(Glaeser,)f(and)g(T.)h(Head-)2145 3068 y(Gordon,)k(J.)g(Chem.)h(Ph)n
635938 > (ys.)f Fh(113)p Fu(\(20\),)f(9140)g(\(2000\).)2042 3133
635939 > y Fn(25)2145 3163 y Fu(A.)h(K.)e(Sop)r(er)h(and)g(M.)g(G.)g(Phillips,)g
635940 > (Chem.)h(Ph)n(ys.)e Fh(107)p Fu(\(1\),)2145 3259 y(47)i(\(1986\).)2042
635941 > 3324 y Fn(26)2145 3354 y Fu(M.)h(Sprik,)g(J.)f(Chem.)h(Ph)n(ys.)e
635942 > Fh(95)p Fu(\(9\),)i(6762)d(\(1991\).)2042 3419 y Fn(27)2145
635943 > 3450 y Fu(A.)36 b(V.)g(Gubsk)-5 b(a)n(y)n(a)35 b(and)g(P)-7
635944 > b(.)35 b(G.)h(Kusalik,)h(J.)e(Chem.)h(Ph)n(ys.)2145 3545
635945 > y Fh(117)p Fu(\(11\),)27 b(5290)f(\(2002\).)2042 3610
635946 > y Fn(28)2145 3641 y Fu(Y.)e(S.)f(Bady)n(al,)g(M.)g(L.)g(Sab)r(oungi,)g
635947 > (D.)h(L.)f(Price,)g(S.)g(D.)h(Shas-)2145 3736 y(tri,)30
635948   b(D.)g(R.)f(Hae\013ner,)g(and)g(A.)h(K.)f(Sop)r(er,)g(J.)g(Chem.)g(Ph)n
635949 < (ys.)2145 3068 y Fg(112)p Ft(\(21\),)e(9206)f(\(2000\).)2042
635950 < 3133 y Fm(28)2145 3163 y Ft(J.)c(Barriol)d(and)j(A.)g(W)-7
635949 > (ys.)2145 3831 y Fh(112)p Fu(\(21\),)e(9206)f(\(2000\).)2042
635950 > 3897 y Fn(29)2145 3927 y Fu(J.)c(Barriol)d(and)j(A.)g(W)-7
635951   b(eisb)r(ec)n(k)n(er,)22 b(Compt.)g(Rend.)g(Acad.)f(Sc.)2145
635952 < 3259 y(P)n(aris)26 b Fg(259)p Ft(,)h(4643)f(\(1964\).)2042
635953 < 3324 y Fm(29)2145 3354 y Ft(B.)32 b(R.)g(Bro)r(oks,)g(R.)g(E.)f
635954 < (Bruccoleri,)h(B.)g(D.)g(Olafson,)g(D.)g(J.)2145 3450
635952 > 4022 y(P)n(aris)26 b Fh(259)p Fu(,)h(4643)f(\(1964\).)2042
635953 > 4088 y Fn(30)2145 4118 y Fu(B.)32 b(R.)g(Bro)r(oks,)g(R.)g(E.)f
635954 > (Bruccoleri,)h(B.)g(D.)g(Olafson,)g(D.)g(J.)2145 4213
635955   y(States,)27 b(S.)f(Sw)n(aminathan,)g(and)g(M.)g(Karplus,)f(J.)h
635956 < (Comput.)2145 3545 y(Chem.)i Fg(4)p Ft(\(2\),)g(187)e(\(1983\).)p
635956 > (Comput.)2145 4309 y(Chem.)i Fh(4)p Fu(\(2\),)g(187)e(\(1983\).)p
635957   eop
635958   %%Trailer
635959   end

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