Supercooled liquids analogous fractional Stokes–Einstein relation in NaCl solution above room temperature
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摘要
The Stokes–Einstein relation D～T/η and its two variants D～τ~(-1) and D～T/τ follow a fractional form in supercooled liquids, where D is the diffusion constant, T the temperature, η the shear viscosity, and τ the structural relaxation time.The fractional Stokes–Einstein relation is proposed to result from the dynamic heterogeneity of supercooled liquids.In this work, by performing molecular dynamics simulations, we show that the analogous fractional form also exists in sodium chloride(NaCl) solutions above room temperature.D～τ~(-1) takes a fractional form within 300–800 K; a crossover is observed in both D～T/τ and D～T/η.Both D～T/τ and D～T/η are valid below the crossover temperature T_x,but take a fractional form for T > T_x.Our results indicate that the fractional Stokes–Einstein relation not only exists in supercooled liquids but also exists in NaCl solutions at high enough temperatures far away from the glass transition point.We propose that D～T/η and its two variants should be critically evaluated to test the validity of the Stokes–Einstein relation.
The Stokes–Einstein relation D～T/η and its two variants D～τ~(-1) and D～T/τ follow a fractional form in supercooled liquids, where D is the diffusion constant, T the temperature, η the shear viscosity, and τ the structural relaxation time.The fractional Stokes–Einstein relation is proposed to result from the dynamic heterogeneity of supercooled liquids.In this work, by performing molecular dynamics simulations, we show that the analogous fractional form also exists in sodium chloride(NaCl) solutions above room temperature.D～τ~(-1) takes a fractional form within 300–800 K; a crossover is observed in both D～T/τ and D～T/η.Both D～T/τ and D～T/η are valid below the crossover temperature T_x,but take a fractional form for T > T_x.Our results indicate that the fractional Stokes–Einstein relation not only exists in supercooled liquids but also exists in NaCl solutions at high enough temperatures far away from the glass transition point.We propose that D～T/η and its two variants should be critically evaluated to test the validity of the Stokes–Einstein relation.
The Stokes–Einstein relation D～T/η and its two variants D～τ~(-1) and D～T/τ follow a fractional form in supercooled liquids, where D is the diffusion constant, T the temperature, η the shear viscosity, and τ the structural relaxation time.The fractional Stokes–Einstein relation is proposed to result from the dynamic heterogeneity of supercooled liquids.In this work, by performing molecular dynamics simulations, we show that the analogous fractional form also exists in sodium chloride(NaCl) solutions above room temperature.D～τ~(-1) takes a fractional form within 300–800 K; a crossover is observed in both D～T/τ and D～T/η.Both D～T/τ and D～T/η are valid below the crossover temperature T_x,but take a fractional form for T > T_x.Our results indicate that the fractional Stokes–Einstein relation not only exists in supercooled liquids but also exists in NaCl solutions at high enough temperatures far away from the glass transition point.We propose that D～T/η and its two variants should be critically evaluated to test the validity of the Stokes–Einstein relation.
引文
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[17]Balatti G, Ambroggio E, Fidelio G, Martini M and Pickholz M 2017Molecules 22 1775
[18]Ishak S, Aris S, Halim K, Ali M, Leow T, Kamarudin N, Masomian M and Rahman R 2017 Molecules 22 1574
[19]Shu C, Xiao K, Cao C, Ding D and Sun X 2017 Molecules 22 1342
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[21]Van Der Spoel D, Lindahl E, Hess B, Groenhof G, Mark A E and Berendsen H J 2005 J.Comput.Chem.26 1701
[22]Brooks B R, Bruccoleri R E, Olafson B D, Swaminathan S and Karplus M 1983 J.Comput.Chem.4 187
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[24]Hassan S A 2008 J.Phys.Chem.B 112 10573
[25]Hassan S A 2008 Phys.Rev.E 77 031501
[26]Hassan S A 2011 J.Chem.Phys.134 114508
[27]Essmann U, Perera L, Berkowitz M L, Darden T, Lee H and Pedersen L G 1995 J.Chem.Phys.103 8577
[28]Nosé S 1984 J.Chem.Phys.81 511
[29]Hoover W G 1985 Phys.Rev.A 31 1695
[30]Lee S H and Rasaiah J C 1994 J.Chem.Phys.101 6964
[31]Anderson J, Ullo J J and Yip S 1987 J.Chem.Phys.87 1726
[32]Bloomfield V, Dalton W and Van Holde K 1967 Biopolymers 5 135
[33]Koneshan S, Rasaiah J C, Lynden-Bell R and Lee S 1998 J.Phys.Chem.B 102 4193
[34]Becker S R, Poole P H and Starr F W 2006 Phys.Rev.Lett.97 055901
[35]Hess B 2002 J.Chem.Phys.116 209
[36]Berthier L 2011 Physics 4 42
[37]Giovambattista N, Mazza M G, Buldyrev S V, Starr F W and Stanley H E 2004 J.Phys.Chem.B 108 6655
[38]Kob W, Donati C, Plimpton S J, Poole P H and Glotzer S C 1997 Phys.Rev.Lett.79 2827
[39]Alder B J and Wainwright T E 1967 Phys.Rev.Lett.18 988
[2]Swallen S F, Bonvallet P A, McMahon R J and Ediger M D 2003 Phys.Rev.Lett.90 015901
[3]Mapes M K, Swallen S F and Ediger M D 2006 J.Phys.Chem.B 110507
[4]Mallamace F, Broccio M, Corsaro C, Faraone A, Wanderlingh U, Liu L, Mou C Y and Chen S H 2006 J.Chem.Phys.124 161102
[5]Xu L, Mallamace F, Yan Z, Starr F W, Buldyrev S V and Eugene Stanley H 2009 Nat.Phys.5 565
[6]Binder K, Kob W, Glassy materials and disordered solids:An introduction to their statistical mechanics World Scientific:2011
[7]Habasaki J, Leon C and Ngai K 2017 Top.Appl.Phys.132
[8]Kumar P, Buldyrev S V, Becker S R, Poole P H, Starr F W and Stanley H E 2007 Proc.Natl.Acad.Sci.104 9575
[9]Jeong D, Choi M Y, Kim H J and Jung Y 2010 Phys.Chem.Chem.Phys.12 2001
[10]Ikeda A and Miyazaki K 2011 Phys.Rev.Lett.106 015701
[11]Grant E H 1957 J.Chem.Phys.26 1575
[12]Varela L M, García M and Mosquera V c 2003 Phys.Rep.382 1
[13]Varela L M, Garcia M and Mosquera V 2003 Phys.Rep.382 1-111
[14]Onsager L and Kim S K 1957 J.Phys.Chem.61 198
[15]Onsager L and Kim S K 1957 J.Phys.Chem.61 198
[16]Vázquez-Raygoza A, Cano-González L, Velázquez-Martínez I, TrejoSoto P, Castillo R, Hernández-Campos A, Hernández-Luis F, OriaHernández J, Castillo-Villanueva A, Avitia-Domínguez C, SierraCampos E, Valdez-Solana M and Téllez-Valencia A 2017 Molecules22 2055
[17]Balatti G, Ambroggio E, Fidelio G, Martini M and Pickholz M 2017Molecules 22 1775
[18]Ishak S, Aris S, Halim K, Ali M, Leow T, Kamarudin N, Masomian M and Rahman R 2017 Molecules 22 1574
[19]Shu C, Xiao K, Cao C, Ding D and Sun X 2017 Molecules 22 1342
[20]Berendsen H J C, van der Spoel D and van Drunen R 1995 Comput.Phys.Commun.91 43
[21]Van Der Spoel D, Lindahl E, Hess B, Groenhof G, Mark A E and Berendsen H J 2005 J.Comput.Chem.26 1701
[22]Brooks B R, Bruccoleri R E, Olafson B D, Swaminathan S and Karplus M 1983 J.Comput.Chem.4 187
[23]Jorgensen W L, Chandrasekhar J, Madura J D, Impey R W and Klein M L 1983 J.Chem.Phys.79 926
[24]Hassan S A 2008 J.Phys.Chem.B 112 10573
[25]Hassan S A 2008 Phys.Rev.E 77 031501
[26]Hassan S A 2011 J.Chem.Phys.134 114508
[27]Essmann U, Perera L, Berkowitz M L, Darden T, Lee H and Pedersen L G 1995 J.Chem.Phys.103 8577
[28]Nosé S 1984 J.Chem.Phys.81 511
[29]Hoover W G 1985 Phys.Rev.A 31 1695
[30]Lee S H and Rasaiah J C 1994 J.Chem.Phys.101 6964
[31]Anderson J, Ullo J J and Yip S 1987 J.Chem.Phys.87 1726
[32]Bloomfield V, Dalton W and Van Holde K 1967 Biopolymers 5 135
[33]Koneshan S, Rasaiah J C, Lynden-Bell R and Lee S 1998 J.Phys.Chem.B 102 4193
[34]Becker S R, Poole P H and Starr F W 2006 Phys.Rev.Lett.97 055901
[35]Hess B 2002 J.Chem.Phys.116 209
[36]Berthier L 2011 Physics 4 42
[37]Giovambattista N, Mazza M G, Buldyrev S V, Starr F W and Stanley H E 2004 J.Phys.Chem.B 108 6655
[38]Kob W, Donati C, Plimpton S J, Poole P H and Glotzer S C 1997 Phys.Rev.Lett.79 2827
[39]Alder B J and Wainwright T E 1967 Phys.Rev.Lett.18 988