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2002
Giovambattista, Nicolas; Starr, Francis W; Sciortino, Francesco; Buldyrev, Sergey V; Stanley, Eugene H
Transitions between inherent structures in water Journal Article
In: PHYSICAL REVIEW E, vol. 65, no. 4, 1, pp. 041502, 2002, ISSN: 1539-3755.
Abstract | BibTeX | Tags: | Links:
@article{ISI:000175146400032b,
title = {Transitions between inherent structures in water},
author = {Nicolas Giovambattista and Francis W Starr and Francesco Sciortino and Sergey V Buldyrev and Eugene H Stanley},
url = {http://fstarr.web.wesleyan.edu/publications/},
doi = {10.1103/PhysRevE.65.041502},
issn = {1539-3755},
year = {2002},
date = {2002-04-01},
journal = {PHYSICAL REVIEW E},
volume = {65},
number = {4, 1},
pages = {041502},
abstract = {The energy landscape approach has been useful to help understand the
dynamic properties of supercooled liquids and the connection between
these properties and thermodynamics. The analysis in numerical models of
the inherent structure (IS) trajectories-the set of local minima visited
by the liquid-offers the possibility of filtering out the vibrational
component of the motion of the system on the potential energy surface
and thereby resolving the slow structural component more efficiently.
Here we report an analysis of an IS trajectory for a widely studied
water model, focusing on the changes in hydrogen bond connectivity that
give rise to many IS's separated by relatively small energy barriers. We
find that while the system travels through these IS's, the structure of
the bond network is continuously modified, exchanging linear bonds for
bifurcated bonds and usually reversing the exchange to return to nearly
the same initial configuration. For the 216-molecule system we
investigate, the time scale of these transitions is as small as the
simulation time scale (approximate to1 fs). Hence, for water, the
transition between each of these IS's is relatively small and eventual
relaxation of the system occurs only by many of these transitions. We
find that during IS changes the molecules with the greatest
displacements move in small ``clusters'' of 1-10 molecules with
displacements of approximate to0.02-0.2 nm, not unlike simpler liquids.
However, for water these clusters appear to be somewhat more branched
than the linear ``stringlike'' clusters formed in a supercooled
Lennard-Jones system found by Glotzer and her collaborators.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The energy landscape approach has been useful to help understand the
dynamic properties of supercooled liquids and the connection between
these properties and thermodynamics. The analysis in numerical models of
the inherent structure (IS) trajectories-the set of local minima visited
by the liquid-offers the possibility of filtering out the vibrational
component of the motion of the system on the potential energy surface
and thereby resolving the slow structural component more efficiently.
Here we report an analysis of an IS trajectory for a widely studied
water model, focusing on the changes in hydrogen bond connectivity that
give rise to many IS's separated by relatively small energy barriers. We
find that while the system travels through these IS's, the structure of
the bond network is continuously modified, exchanging linear bonds for
bifurcated bonds and usually reversing the exchange to return to nearly
the same initial configuration. For the 216-molecule system we
investigate, the time scale of these transitions is as small as the
simulation time scale (approximate to1 fs). Hence, for water, the
transition between each of these IS's is relatively small and eventual
relaxation of the system occurs only by many of these transitions. We
find that during IS changes the molecules with the greatest
displacements move in small ``clusters'' of 1-10 molecules with
displacements of approximate to0.02-0.2 nm, not unlike simpler liquids.
However, for water these clusters appear to be somewhat more branched
than the linear ``stringlike'' clusters formed in a supercooled
Lennard-Jones system found by Glotzer and her collaborators.
dynamic properties of supercooled liquids and the connection between
these properties and thermodynamics. The analysis in numerical models of
the inherent structure (IS) trajectories-the set of local minima visited
by the liquid-offers the possibility of filtering out the vibrational
component of the motion of the system on the potential energy surface
and thereby resolving the slow structural component more efficiently.
Here we report an analysis of an IS trajectory for a widely studied
water model, focusing on the changes in hydrogen bond connectivity that
give rise to many IS's separated by relatively small energy barriers. We
find that while the system travels through these IS's, the structure of
the bond network is continuously modified, exchanging linear bonds for
bifurcated bonds and usually reversing the exchange to return to nearly
the same initial configuration. For the 216-molecule system we
investigate, the time scale of these transitions is as small as the
simulation time scale (approximate to1 fs). Hence, for water, the
transition between each of these IS's is relatively small and eventual
relaxation of the system occurs only by many of these transitions. We
find that during IS changes the molecules with the greatest
displacements move in small ``clusters'' of 1-10 molecules with
displacements of approximate to0.02-0.2 nm, not unlike simpler liquids.
However, for water these clusters appear to be somewhat more branched
than the linear ``stringlike'' clusters formed in a supercooled
Lennard-Jones system found by Glotzer and her collaborators.
Stanley, H. Eugene; Buldyrev, Sergey V.; Giovambattista, Nicolas; La Nave, Emilia; Scala, Antonio; Sciortino, Francesco; Starr, Francis W.
Statistical physics and liquid water: ``What matters'' Journal Article
In: PHYSICA A-STATISTICAL MECHANICS AND ITS APPLICATIONS, vol. 306, no. 1-4, pp. 230-242, 2002, ISSN: 0378-4371, (21st IUPAP International Conference on Statistical Physics, CANCUN, MEXICO, JUL 15-21, 2001).
Abstract | BibTeX | Tags: | Links:
@article{ISI:000175781700025,
title = {Statistical physics and liquid water: ``What matters''},
author = {Stanley, H. Eugene and Buldyrev, Sergey V. and Giovambattista, Nicolas and La Nave, Emilia and Scala, Antonio and Sciortino, Francesco and Starr, Francis W.},
url = {http://fstarr.web.wesleyan.edu/publications/},
doi = {10.1016/S0378-4371(02)00544-7},
issn = {0378-4371},
year = {2002},
date = {2002-04-01},
journal = {PHYSICA A-STATISTICAL MECHANICS AND ITS APPLICATIONS},
volume = {306},
number = {1-4},
pages = {230-242},
abstract = {We present an over-view of recent research applying ideas of statistical mechanics to try to better understand the statics and especially the dynamic puzzles regarding liquid water. The take-home message for the static aspects is that what seems to ``matter'' more than previously appreciated is local tetrahedral order, so that liquid water has features in common with SiO(2) and P, as well as perhaps Si and C. For the dynamic aspects, what may ``matter'' is the number of diffusive directions in the potential energy landscape. (C) 2002 Published by Elsevier Science B.V.},
note = {21st IUPAP International Conference on Statistical Physics, CANCUN, MEXICO, JUL 15-21, 2001},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We present an over-view of recent research applying ideas of statistical mechanics to try to better understand the statics and especially the dynamic puzzles regarding liquid water. The take-home message for the static aspects is that what seems to ``matter'' more than previously appreciated is local tetrahedral order, so that liquid water has features in common with SiO(2) and P, as well as perhaps Si and C. For the dynamic aspects, what may ``matter'' is the number of diffusive directions in the potential energy landscape. (C) 2002 Published by Elsevier Science B.V.
Giovambattista, Nicolas; Starr, Francis W.; Sciortino, Francesco; Buldyrev, Sergey V.; Stanley, H. Eugene
Transitions between inherent structures in water Journal Article
In: PHYSICAL REVIEW E, vol. 65, no. 4, 1, pp. 041502, 2002, ISSN: 1539-3755.
Abstract | BibTeX | Tags: | Links:
@article{ISI:000175146400032,
title = {Transitions between inherent structures in water},
author = {Giovambattista, Nicolas and Starr, Francis W. and Sciortino, Francesco and Buldyrev, Sergey V. and Stanley, H. Eugene},
url = {http://fstarr.web.wesleyan.edu/publications/},
doi = {10.1103/PhysRevE.65.041502},
issn = {1539-3755},
year = {2002},
date = {2002-04-01},
journal = {PHYSICAL REVIEW E},
volume = {65},
number = {4, 1},
pages = {041502},
abstract = {The energy landscape approach has been useful to help understand the dynamic properties of supercooled liquids and the connection between these properties and thermodynamics. The analysis in numerical models of the inherent structure (IS) trajectories-the set of local minima visited by the liquid-offers the possibility of filtering out the vibrational component of the motion of the system on the potential energy surface and thereby resolving the slow structural component more efficiently. Here we report an analysis of an IS trajectory for a widely studied water model, focusing on the changes in hydrogen bond connectivity that give rise to many IS's separated by relatively small energy barriers. We find that while the system travels through these IS's, the structure of the bond network is continuously modified, exchanging linear bonds for bifurcated bonds and usually reversing the exchange to return to nearly the same initial configuration. For the 216-molecule system we investigate, the time scale of these transitions is as small as the simulation time scale (approximate to1 fs). Hence, for water, the transition between each of these IS's is relatively small and eventual relaxation of the system occurs only by many of these transitions. We find that during IS changes the molecules with the greatest displacements move in small ``clusters'' of 1-10 molecules with displacements of approximate to0.02-0.2 nm, not unlike simpler liquids. However, for water these clusters appear to be somewhat more branched than the linear ``stringlike'' clusters formed in a supercooled Lennard-Jones system found by Glotzer and her collaborators.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The energy landscape approach has been useful to help understand the dynamic properties of supercooled liquids and the connection between these properties and thermodynamics. The analysis in numerical models of the inherent structure (IS) trajectories-the set of local minima visited by the liquid-offers the possibility of filtering out the vibrational component of the motion of the system on the potential energy surface and thereby resolving the slow structural component more efficiently. Here we report an analysis of an IS trajectory for a widely studied water model, focusing on the changes in hydrogen bond connectivity that give rise to many IS's separated by relatively small energy barriers. We find that while the system travels through these IS's, the structure of the bond network is continuously modified, exchanging linear bonds for bifurcated bonds and usually reversing the exchange to return to nearly the same initial configuration. For the 216-molecule system we investigate, the time scale of these transitions is as small as the simulation time scale (approximate to1 fs). Hence, for water, the transition between each of these IS's is relatively small and eventual relaxation of the system occurs only by many of these transitions. We find that during IS changes the molecules with the greatest displacements move in small ``clusters'' of 1-10 molecules with displacements of approximate to0.02-0.2 nm, not unlike simpler liquids. However, for water these clusters appear to be somewhat more branched than the linear ``stringlike'' clusters formed in a supercooled Lennard-Jones system found by Glotzer and her collaborators.
2001
Gebremichael, Yeshitila; Schrøder, Thomas B; Starr, Francis W; Glotzer, Sharon C
Spatially correlated dynamics in a simulated glass-forming polymer melt: Analysis of clustering phenomena Journal Article
In: PHYSICAL REVIEW E, vol. 64, no. 5, 1, pp. 051503, 2001, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{gssg01b,
title = {Spatially correlated dynamics in a simulated glass-forming polymer melt:
Analysis of clustering phenomena},
author = {Yeshitila Gebremichael and Thomas B Schrøder and Francis W Starr and Sharon C Glotzer},
url = {http://fstarr.web.wesleyan.edu/publications/gssg.pdf},
doi = {10.1103/PhysRevE.64.051503},
issn = {1063-651X},
year = {2001},
date = {2001-11-01},
journal = {PHYSICAL REVIEW E},
volume = {64},
number = {5, 1},
pages = {051503},
abstract = {In recent years. experimental and computational studies have
demonstrated that the dynamics of glass-forming liquids are spatially
heterogeneous, exhibiting regions of temporarily enhanced or diminished
mobility. Here we present a detailed analysis of dynamical heterogeneity
in a simulated ``bead-spring'' model of a low-molecular-weight polymer
melt. We investigate the transient nature and size distribution of
clusters of ``mobile'' chain segments (monomers) as the polymer melt
is cooled toward its glass transition. We also explore the dependence of
this clustering on the way in which the mobile subset is defined, We
show that the mean cluster size is time dependent with a peak at
intermediate time, and that the mean cluster size at the peak time.-rows
with decreasing temperature T. We show that for each T a particular
fraction of particles maximizes the mean cluster size at some
characteristic time, and this fraction depends on T, The growing size of
the clusters demonstrates the growing range of correlated motion,
previously reported for this same system [C. Beneman et al. Nature
(London) 399, 246 (1999)]. The distribution of cluster sizes approaches
a power law near the mode-coupling temperature, similar to behavior
reported for a simulated binary mixture and a dense colloidal
suspension, but with a different exponent, We calculate the correlation
length of the clusters, and show that it exhibits similar temperature-
and time-dependent behavior as the mean cluster size, with a maximum at
intermediate time. We show that the characteristic time of the maximum
cluster size follows the scaling predicted by mode-coupling theory (MCT)
for the beta time scale, revealing a possible connection between
spatially heterogeneous dynamics and MCT.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
In recent years. experimental and computational studies have
demonstrated that the dynamics of glass-forming liquids are spatially
heterogeneous, exhibiting regions of temporarily enhanced or diminished
mobility. Here we present a detailed analysis of dynamical heterogeneity
in a simulated ``bead-spring'' model of a low-molecular-weight polymer
melt. We investigate the transient nature and size distribution of
clusters of ``mobile'' chain segments (monomers) as the polymer melt
is cooled toward its glass transition. We also explore the dependence of
this clustering on the way in which the mobile subset is defined, We
show that the mean cluster size is time dependent with a peak at
intermediate time, and that the mean cluster size at the peak time.-rows
with decreasing temperature T. We show that for each T a particular
fraction of particles maximizes the mean cluster size at some
characteristic time, and this fraction depends on T, The growing size of
the clusters demonstrates the growing range of correlated motion,
previously reported for this same system [C. Beneman et al. Nature
(London) 399, 246 (1999)]. The distribution of cluster sizes approaches
a power law near the mode-coupling temperature, similar to behavior
reported for a simulated binary mixture and a dense colloidal
suspension, but with a different exponent, We calculate the correlation
length of the clusters, and show that it exhibits similar temperature-
and time-dependent behavior as the mean cluster size, with a maximum at
intermediate time. We show that the characteristic time of the maximum
cluster size follows the scaling predicted by mode-coupling theory (MCT)
for the beta time scale, revealing a possible connection between
spatially heterogeneous dynamics and MCT.
demonstrated that the dynamics of glass-forming liquids are spatially
heterogeneous, exhibiting regions of temporarily enhanced or diminished
mobility. Here we present a detailed analysis of dynamical heterogeneity
in a simulated ``bead-spring'' model of a low-molecular-weight polymer
melt. We investigate the transient nature and size distribution of
clusters of ``mobile'' chain segments (monomers) as the polymer melt
is cooled toward its glass transition. We also explore the dependence of
this clustering on the way in which the mobile subset is defined, We
show that the mean cluster size is time dependent with a peak at
intermediate time, and that the mean cluster size at the peak time.-rows
with decreasing temperature T. We show that for each T a particular
fraction of particles maximizes the mean cluster size at some
characteristic time, and this fraction depends on T, The growing size of
the clusters demonstrates the growing range of correlated motion,
previously reported for this same system [C. Beneman et al. Nature
(London) 399, 246 (1999)]. The distribution of cluster sizes approaches
a power law near the mode-coupling temperature, similar to behavior
reported for a simulated binary mixture and a dense colloidal
suspension, but with a different exponent, We calculate the correlation
length of the clusters, and show that it exhibits similar temperature-
and time-dependent behavior as the mean cluster size, with a maximum at
intermediate time. We show that the characteristic time of the maximum
cluster size follows the scaling predicted by mode-coupling theory (MCT)
for the beta time scale, revealing a possible connection between
spatially heterogeneous dynamics and MCT.
Gebremichael, Yeshitila; Schrøder, Thomas B.; Starr, Francis W.; Glotzer, Sharon C.
Spatially correlated dynamics in a simulated glass-forming polymer melt: Analysis of clustering phenomena Journal Article
In: PHYSICAL REVIEW E, vol. 64, no. 5, 1, pp. 051503, 2001, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{gssg01,
title = {Spatially correlated dynamics in a simulated glass-forming polymer melt: Analysis of clustering phenomena},
author = {Gebremichael, Yeshitila and Schrøder, Thomas B. and Starr, Francis W. and Glotzer, Sharon C.},
url = {http://fstarr.web.wesleyan.edu/publications/gssg.pdf},
doi = {10.1103/PhysRevE.64.051503},
issn = {1063-651X},
year = {2001},
date = {2001-11-01},
journal = {PHYSICAL REVIEW E},
volume = {64},
number = {5, 1},
pages = {051503},
abstract = {In recent years. experimental and computational studies have demonstrated that the dynamics of glass-forming liquids are spatially heterogeneous, exhibiting regions of temporarily enhanced or diminished mobility. Here we present a detailed analysis of dynamical heterogeneity in a simulated ``bead-spring'' model of a low-molecular-weight polymer melt. We investigate the transient nature and size distribution of clusters of ``mobile'' chain segments (monomers) as the polymer melt is cooled toward its glass transition. We also explore the dependence of this clustering on the way in which the mobile subset is defined, We show that the mean cluster size is time dependent with a peak at intermediate time, and that the mean cluster size at the peak time.-rows with decreasing temperature T. We show that for each T a particular fraction of particles maximizes the mean cluster size at some characteristic time, and this fraction depends on T, The growing size of the clusters demonstrates the growing range of correlated motion, previously reported for this same system [C. Beneman et al. Nature (London) 399, 246 (1999)]. The distribution of cluster sizes approaches a power law near the mode-coupling temperature, similar to behavior reported for a simulated binary mixture and a dense colloidal suspension, but with a different exponent, We calculate the correlation length of the clusters, and show that it exhibits similar temperature- and time-dependent behavior as the mean cluster size, with a maximum at intermediate time. We show that the characteristic time of the maximum cluster size follows the scaling predicted by mode-coupling theory (MCT) for the beta time scale, revealing a possible connection between spatially heterogeneous dynamics and MCT.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
In recent years. experimental and computational studies have demonstrated that the dynamics of glass-forming liquids are spatially heterogeneous, exhibiting regions of temporarily enhanced or diminished mobility. Here we present a detailed analysis of dynamical heterogeneity in a simulated ``bead-spring'' model of a low-molecular-weight polymer melt. We investigate the transient nature and size distribution of clusters of ``mobile'' chain segments (monomers) as the polymer melt is cooled toward its glass transition. We also explore the dependence of this clustering on the way in which the mobile subset is defined, We show that the mean cluster size is time dependent with a peak at intermediate time, and that the mean cluster size at the peak time.-rows with decreasing temperature T. We show that for each T a particular fraction of particles maximizes the mean cluster size at some characteristic time, and this fraction depends on T, The growing size of the clusters demonstrates the growing range of correlated motion, previously reported for this same system [C. Beneman et al. Nature (London) 399, 246 (1999)]. The distribution of cluster sizes approaches a power law near the mode-coupling temperature, similar to behavior reported for a simulated binary mixture and a dense colloidal suspension, but with a different exponent, We calculate the correlation length of the clusters, and show that it exhibits similar temperature- and time-dependent behavior as the mean cluster size, with a maximum at intermediate time. We show that the characteristic time of the maximum cluster size follows the scaling predicted by mode-coupling theory (MCT) for the beta time scale, revealing a possible connection between spatially heterogeneous dynamics and MCT.
Nave, Emilia La; Scala, Antonio; Starr, Francis W; Stanley, Eugene H; Sciortino, F
Dynamics of supercooled water in configuration space Journal Article
In: PHYSICAL REVIEW E, vol. 64, no. 3, 2, pp. 036102, 2001, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{lssss01b,
title = {Dynamics of supercooled water in configuration space},
author = {Emilia La Nave and Antonio Scala and Francis W Starr and Eugene H Stanley and F Sciortino},
url = {http://fstarr.web.wesleyan.edu/publications/lssss-pre.pdf},
doi = {10.1103/PhysRevE.64.036102},
issn = {1063-651X},
year = {2001},
date = {2001-09-01},
journal = {PHYSICAL REVIEW E},
volume = {64},
number = {3, 2},
pages = {036102},
abstract = {We study the potential energy surface (PES) sampled by a liquid modeled
via the widely studied extended simple point charge (SPC/E) model for
water. We characterize the curvature of the PES by calculating the
instantaneous normal mode (INM) spectrum for a wide range of densities
and temperatures. We discuss the information contained in the INM
density of states, which requires additional processing to be
unambiguously associated with the long-time dynamics. For the SPC/E
model, we find that the slowing down of the dynamics in the supercooled
region-where the ideal mode coupling theory has been used to describe
the dynamics-is controlled by the reduction in the number of directions
in configuration space that allow a structural change. We find that the
fraction fd, of the double-well directions in configuration space
determines the value of the diffusion constant D, thereby relating a
property of the PES to a macroscopic dynamic quantity; specifically, it
appears that rootD is approximately linear in f(dw). Our findings are
consistent with the hypothesis that, at the mode coupling crossover
temperature, dynamical processes based on the free exploration of
configuration space vanish, and processes requiring activation dominate.
Hence, the reduction of the number of directions allowing free
exploration of configuration space is the mechanism of diffusion
implicitly implemented in the ideal mode coupling theory. Additionally,
we find a direct relationship between the number of basins sampled by
the system and the number of free directions. In this picture, diffusion
appears to be related to geometrical properties of the PES, and to be
entropic in origin.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We study the potential energy surface (PES) sampled by a liquid modeled
via the widely studied extended simple point charge (SPC/E) model for
water. We characterize the curvature of the PES by calculating the
instantaneous normal mode (INM) spectrum for a wide range of densities
and temperatures. We discuss the information contained in the INM
density of states, which requires additional processing to be
unambiguously associated with the long-time dynamics. For the SPC/E
model, we find that the slowing down of the dynamics in the supercooled
region-where the ideal mode coupling theory has been used to describe
the dynamics-is controlled by the reduction in the number of directions
in configuration space that allow a structural change. We find that the
fraction fd, of the double-well directions in configuration space
determines the value of the diffusion constant D, thereby relating a
property of the PES to a macroscopic dynamic quantity; specifically, it
appears that rootD is approximately linear in f(dw). Our findings are
consistent with the hypothesis that, at the mode coupling crossover
temperature, dynamical processes based on the free exploration of
configuration space vanish, and processes requiring activation dominate.
Hence, the reduction of the number of directions allowing free
exploration of configuration space is the mechanism of diffusion
implicitly implemented in the ideal mode coupling theory. Additionally,
we find a direct relationship between the number of basins sampled by
the system and the number of free directions. In this picture, diffusion
appears to be related to geometrical properties of the PES, and to be
entropic in origin.
via the widely studied extended simple point charge (SPC/E) model for
water. We characterize the curvature of the PES by calculating the
instantaneous normal mode (INM) spectrum for a wide range of densities
and temperatures. We discuss the information contained in the INM
density of states, which requires additional processing to be
unambiguously associated with the long-time dynamics. For the SPC/E
model, we find that the slowing down of the dynamics in the supercooled
region-where the ideal mode coupling theory has been used to describe
the dynamics-is controlled by the reduction in the number of directions
in configuration space that allow a structural change. We find that the
fraction fd, of the double-well directions in configuration space
determines the value of the diffusion constant D, thereby relating a
property of the PES to a macroscopic dynamic quantity; specifically, it
appears that rootD is approximately linear in f(dw). Our findings are
consistent with the hypothesis that, at the mode coupling crossover
temperature, dynamical processes based on the free exploration of
configuration space vanish, and processes requiring activation dominate.
Hence, the reduction of the number of directions allowing free
exploration of configuration space is the mechanism of diffusion
implicitly implemented in the ideal mode coupling theory. Additionally,
we find a direct relationship between the number of basins sampled by
the system and the number of free directions. In this picture, diffusion
appears to be related to geometrical properties of the PES, and to be
entropic in origin.
La Nave, Emilia; Scala, Antonio; Starr, Francis W.; Stanley, H. Eugene; Sciortino, F
Dynamics of supercooled water in configuration space Journal Article
In: PHYSICAL REVIEW E, vol. 64, no. 3, 2, pp. 036102, 2001, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{lssss01,
title = {Dynamics of supercooled water in configuration space},
author = {La Nave, Emilia and Scala, Antonio and Starr, Francis W. and Stanley, H. Eugene and Sciortino, F},
url = {http://fstarr.web.wesleyan.edu/publications/lssss-pre.pdf},
doi = {10.1103/PhysRevE.64.036102},
issn = {1063-651X},
year = {2001},
date = {2001-09-01},
journal = {PHYSICAL REVIEW E},
volume = {64},
number = {3, 2},
pages = {036102},
abstract = {We study the potential energy surface (PES) sampled by a liquid modeled via the widely studied extended simple point charge (SPC/E) model for water. We characterize the curvature of the PES by calculating the instantaneous normal mode (INM) spectrum for a wide range of densities and temperatures. We discuss the information contained in the INM density of states, which requires additional processing to be unambiguously associated with the long-time dynamics. For the SPC/E model, we find that the slowing down of the dynamics in the supercooled region-where the ideal mode coupling theory has been used to describe the dynamics-is controlled by the reduction in the number of directions in configuration space that allow a structural change. We find that the fraction fd, of the double-well directions in configuration space determines the value of the diffusion constant D, thereby relating a property of the PES to a macroscopic dynamic quantity; specifically, it appears that rootD is approximately linear in f(dw). Our findings are consistent with the hypothesis that, at the mode coupling crossover temperature, dynamical processes based on the free exploration of configuration space vanish, and processes requiring activation dominate. Hence, the reduction of the number of directions allowing free exploration of configuration space is the mechanism of diffusion implicitly implemented in the ideal mode coupling theory. Additionally, we find a direct relationship between the number of basins sampled by the system and the number of free directions. In this picture, diffusion appears to be related to geometrical properties of the PES, and to be entropic in origin.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We study the potential energy surface (PES) sampled by a liquid modeled via the widely studied extended simple point charge (SPC/E) model for water. We characterize the curvature of the PES by calculating the instantaneous normal mode (INM) spectrum for a wide range of densities and temperatures. We discuss the information contained in the INM density of states, which requires additional processing to be unambiguously associated with the long-time dynamics. For the SPC/E model, we find that the slowing down of the dynamics in the supercooled region-where the ideal mode coupling theory has been used to describe the dynamics-is controlled by the reduction in the number of directions in configuration space that allow a structural change. We find that the fraction fd, of the double-well directions in configuration space determines the value of the diffusion constant D, thereby relating a property of the PES to a macroscopic dynamic quantity; specifically, it appears that rootD is approximately linear in f(dw). Our findings are consistent with the hypothesis that, at the mode coupling crossover temperature, dynamical processes based on the free exploration of configuration space vanish, and processes requiring activation dominate. Hence, the reduction of the number of directions allowing free exploration of configuration space is the mechanism of diffusion implicitly implemented in the ideal mode coupling theory. Additionally, we find a direct relationship between the number of basins sampled by the system and the number of free directions. In this picture, diffusion appears to be related to geometrical properties of the PES, and to be entropic in origin.
Starr, Francis W; Schrøder, Thomas B; Glotzer, Sharon C
Effects of a nanoscopic filler on the structure and dynamics of a simulated polymer melt and the relationship to ultrathin films Journal Article
In: PHYSICAL REVIEW E, vol. 64, no. 2, 1, pp. 021802, 2001, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{ssg01d,
title = {Effects of a nanoscopic filler on the structure and dynamics of a
simulated polymer melt and the relationship to ultrathin films},
author = {Francis W Starr and Thomas B Schrøder and Sharon C Glotzer},
url = {http://fstarr.web.wesleyan.edu/publications/ssg-pre.pdf},
doi = {10.1103/PhysRevE.64.021802},
issn = {1063-651X},
year = {2001},
date = {2001-08-01},
journal = {PHYSICAL REVIEW E},
volume = {64},
number = {2, 1},
pages = {021802},
abstract = {We perform molecular dynamics simulations of an idealized polymer melt
surrounding a nanoscopic filler particle. We show that the glass
transition temperature T-g of the melt can be shifted to either higher
or lower temperatures by tuning the interactions between polymer and
filler. A gradual change of the polymer dynamics approaching the filler
surface causes the change in the glass transition. We also find that
polymers close to the surface tend to be elongated and flattened. Our
findings show a strong similarity to those obtained for ultrathin
polymer films.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We perform molecular dynamics simulations of an idealized polymer melt
surrounding a nanoscopic filler particle. We show that the glass
transition temperature T-g of the melt can be shifted to either higher
or lower temperatures by tuning the interactions between polymer and
filler. A gradual change of the polymer dynamics approaching the filler
surface causes the change in the glass transition. We also find that
polymers close to the surface tend to be elongated and flattened. Our
findings show a strong similarity to those obtained for ultrathin
polymer films.
surrounding a nanoscopic filler particle. We show that the glass
transition temperature T-g of the melt can be shifted to either higher
or lower temperatures by tuning the interactions between polymer and
filler. A gradual change of the polymer dynamics approaching the filler
surface causes the change in the glass transition. We also find that
polymers close to the surface tend to be elongated and flattened. Our
findings show a strong similarity to those obtained for ultrathin
polymer films.
Starr, Francis W.; Schrøder, Thomas B.; Glotzer, Sharon C.
Effects of a nanoscopic filler on the structure and dynamics of a simulated polymer melt and the relationship to ultrathin films Journal Article
In: PHYSICAL REVIEW E, vol. 64, no. 2, 1, pp. 021802, 2001, ISSN: 1063-651X.
Abstract | BibTeX | Tags: Glass Formation, Nanocomposites, Polymers | Links:
@article{ssg01,
title = {Effects of a nanoscopic filler on the structure and dynamics of a simulated polymer melt and the relationship to ultrathin films},
author = {Starr, Francis W. and Schrøder, Thomas B. and Glotzer, Sharon C.},
url = {http://fstarr.web.wesleyan.edu/publications/ssg-pre.pdf},
doi = {10.1103/PhysRevE.64.021802},
issn = {1063-651X},
year = {2001},
date = {2001-08-01},
journal = {PHYSICAL REVIEW E},
volume = {64},
number = {2, 1},
pages = {021802},
abstract = {We perform molecular dynamics simulations of an idealized polymer melt surrounding a nanoscopic filler particle. We show that the glass transition temperature T-g of the melt can be shifted to either higher or lower temperatures by tuning the interactions between polymer and filler. A gradual change of the polymer dynamics approaching the filler surface causes the change in the glass transition. We also find that polymers close to the surface tend to be elongated and flattened. Our findings show a strong similarity to those obtained for ultrathin polymer films.},
keywords = {Glass Formation, Nanocomposites, Polymers},
pubstate = {published},
tppubtype = {article}
}
We perform molecular dynamics simulations of an idealized polymer melt surrounding a nanoscopic filler particle. We show that the glass transition temperature T-g of the melt can be shifted to either higher or lower temperatures by tuning the interactions between polymer and filler. A gradual change of the polymer dynamics approaching the filler surface causes the change in the glass transition. We also find that polymers close to the surface tend to be elongated and flattened. Our findings show a strong similarity to those obtained for ultrathin polymer films.
Netz, Paulo A; Starr, Francis W; Stanley, Eugene H; Barbosa, Marcia C
Static and dynamic properties of stretched water Journal Article
In: JOURNAL OF CHEMICAL PHYSICS, vol. 115, no. 1, pp. 344-348, 2001, ISSN: 0021-9606.
Abstract | BibTeX | Tags: | Links:
@article{nssb01b,
title = {Static and dynamic properties of stretched water},
author = {Paulo A Netz and Francis W Starr and Eugene H Stanley and Marcia C Barbosa},
url = {http://fstarr.web.wesleyan.edu/publications/nssb.pdf},
doi = {10.1063/1.1376424},
issn = {0021-9606},
year = {2001},
date = {2001-07-01},
journal = {JOURNAL OF CHEMICAL PHYSICS},
volume = {115},
number = {1},
pages = {344-348},
abstract = {We present the results of molecular dynamics simulations of the extended
simple point charge model of water to investigate the thermodynamic and
dynamic properties of stretched and supercooled water. We locate the
liquid-gas spinodal, and confirm that the spinodal pressure increases
monotonically with T, supporting thermodynamic scenarios for the phase
behavior of supercooled water involving a ``non-reentrant'' spinodal.
The dynamics at negative pressure show a minimum in the diffusion
constant D when the density is decreased at constant temperature,
complementary to the known maximum of D at higher pressures. We locate
the loci of minima of D relative to the spinodal, showing that the locus
is inside the thermodynamically metastable regions of the phase diagram.
These dynamical results reflect the initial enhancement and subsequent
breakdown of the tetrahedral structure and of the hydrogen bond network
as the density decreases. (C) 2001 American Institute of Physics.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We present the results of molecular dynamics simulations of the extended
simple point charge model of water to investigate the thermodynamic and
dynamic properties of stretched and supercooled water. We locate the
liquid-gas spinodal, and confirm that the spinodal pressure increases
monotonically with T, supporting thermodynamic scenarios for the phase
behavior of supercooled water involving a ``non-reentrant'' spinodal.
The dynamics at negative pressure show a minimum in the diffusion
constant D when the density is decreased at constant temperature,
complementary to the known maximum of D at higher pressures. We locate
the loci of minima of D relative to the spinodal, showing that the locus
is inside the thermodynamically metastable regions of the phase diagram.
These dynamical results reflect the initial enhancement and subsequent
breakdown of the tetrahedral structure and of the hydrogen bond network
as the density decreases. (C) 2001 American Institute of Physics.
simple point charge model of water to investigate the thermodynamic and
dynamic properties of stretched and supercooled water. We locate the
liquid-gas spinodal, and confirm that the spinodal pressure increases
monotonically with T, supporting thermodynamic scenarios for the phase
behavior of supercooled water involving a ``non-reentrant'' spinodal.
The dynamics at negative pressure show a minimum in the diffusion
constant D when the density is decreased at constant temperature,
complementary to the known maximum of D at higher pressures. We locate
the loci of minima of D relative to the spinodal, showing that the locus
is inside the thermodynamically metastable regions of the phase diagram.
These dynamical results reflect the initial enhancement and subsequent
breakdown of the tetrahedral structure and of the hydrogen bond network
as the density decreases. (C) 2001 American Institute of Physics.
Netz, Paulo A.; Starr, Francis W.; Stanley, H. Eugene; Barbosa, Marcia C.
Static and dynamic properties of stretched water Journal Article
In: JOURNAL OF CHEMICAL PHYSICS, vol. 115, no. 1, pp. 344-348, 2001, ISSN: 0021-9606.
Abstract | BibTeX | Tags: | Links:
@article{nssb01,
title = {Static and dynamic properties of stretched water},
author = {Netz, Paulo A. and Starr, Francis W. and Stanley, H. Eugene and Barbosa, Marcia C.},
url = {http://fstarr.web.wesleyan.edu/publications/nssb.pdf},
doi = {10.1063/1.1376424},
issn = {0021-9606},
year = {2001},
date = {2001-07-01},
journal = {JOURNAL OF CHEMICAL PHYSICS},
volume = {115},
number = {1},
pages = {344-348},
abstract = {We present the results of molecular dynamics simulations of the extended simple point charge model of water to investigate the thermodynamic and dynamic properties of stretched and supercooled water. We locate the liquid-gas spinodal, and confirm that the spinodal pressure increases monotonically with T, supporting thermodynamic scenarios for the phase behavior of supercooled water involving a ``non-reentrant'' spinodal. The dynamics at negative pressure show a minimum in the diffusion constant D when the density is decreased at constant temperature, complementary to the known maximum of D at higher pressures. We locate the loci of minima of D relative to the spinodal, showing that the locus is inside the thermodynamically metastable regions of the phase diagram. These dynamical results reflect the initial enhancement and subsequent breakdown of the tetrahedral structure and of the hydrogen bond network as the density decreases. (C) 2001 American Institute of Physics.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We present the results of molecular dynamics simulations of the extended simple point charge model of water to investigate the thermodynamic and dynamic properties of stretched and supercooled water. We locate the liquid-gas spinodal, and confirm that the spinodal pressure increases monotonically with T, supporting thermodynamic scenarios for the phase behavior of supercooled water involving a ``non-reentrant'' spinodal. The dynamics at negative pressure show a minimum in the diffusion constant D when the density is decreased at constant temperature, complementary to the known maximum of D at higher pressures. We locate the loci of minima of D relative to the spinodal, showing that the locus is inside the thermodynamically metastable regions of the phase diagram. These dynamical results reflect the initial enhancement and subsequent breakdown of the tetrahedral structure and of the hydrogen bond network as the density decreases. (C) 2001 American Institute of Physics.
Starr, Francis W; Sastry, Srikanth; Nave, Emilia La; Scala, Antonio; Stanley, Eugene H; Sciortino, F
Thermodynamic and structural aspects of the potential energy surface of simulated water Journal Article
In: PHYSICAL REVIEW E, vol. 63, no. 4, 1, pp. 041201, 2001, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{sslsss01b,
title = {Thermodynamic and structural aspects of the potential energy surface of
simulated water},
author = {Francis W Starr and Srikanth Sastry and Emilia La Nave and Antonio Scala and Eugene H Stanley and F Sciortino},
url = {http://fstarr.web.wesleyan.edu/publications/sslsss.pdf},
doi = {10.1103/PhysRevE.63.041201},
issn = {1063-651X},
year = {2001},
date = {2001-04-01},
journal = {PHYSICAL REVIEW E},
volume = {63},
number = {4, 1},
pages = {041201},
abstract = {Relations between the thermodynamics and dynamics of supercooled liquids
approaching a glass transition is a topic of considerable interest. The
potential energy surface of model liquids has been increasingly studied,
since it provides a connection between the configurational component of
the partition function on the one hand, and the system dynamics on the
other. This connection is most obvious at low temperatures, where the
motion of the system can be partitioned into vibrations within a basin
of attraction and infrequent interbasin transitions. in this work, we
present a description of the potential energy surface properties of
supercooled liquid water. The dynamics of this model have been studied
in great detail in recent years. We locate the minima sampled by the
liquid by ``quenches'' from equilibrium configurations generated via
molecular dynamics simulations, and then calculate the temperature and
density dependence of the basin energy, degeneracy, and shape. The
temperature dependence of the energy of the minima is qualitatively
similar to simple liquids, but has anomalous density dependence. The
unusual density dependence is also reflected in the configurational
entropy, the thermodynamic measure of degeneracy. Finally, we study the
structure of simulated water at the minima, which provides insight on
the progressive tetrahedral ordering of the liquid on cooling.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Relations between the thermodynamics and dynamics of supercooled liquids
approaching a glass transition is a topic of considerable interest. The
potential energy surface of model liquids has been increasingly studied,
since it provides a connection between the configurational component of
the partition function on the one hand, and the system dynamics on the
other. This connection is most obvious at low temperatures, where the
motion of the system can be partitioned into vibrations within a basin
of attraction and infrequent interbasin transitions. in this work, we
present a description of the potential energy surface properties of
supercooled liquid water. The dynamics of this model have been studied
in great detail in recent years. We locate the minima sampled by the
liquid by ``quenches'' from equilibrium configurations generated via
molecular dynamics simulations, and then calculate the temperature and
density dependence of the basin energy, degeneracy, and shape. The
temperature dependence of the energy of the minima is qualitatively
similar to simple liquids, but has anomalous density dependence. The
unusual density dependence is also reflected in the configurational
entropy, the thermodynamic measure of degeneracy. Finally, we study the
structure of simulated water at the minima, which provides insight on
the progressive tetrahedral ordering of the liquid on cooling.
approaching a glass transition is a topic of considerable interest. The
potential energy surface of model liquids has been increasingly studied,
since it provides a connection between the configurational component of
the partition function on the one hand, and the system dynamics on the
other. This connection is most obvious at low temperatures, where the
motion of the system can be partitioned into vibrations within a basin
of attraction and infrequent interbasin transitions. in this work, we
present a description of the potential energy surface properties of
supercooled liquid water. The dynamics of this model have been studied
in great detail in recent years. We locate the minima sampled by the
liquid by ``quenches'' from equilibrium configurations generated via
molecular dynamics simulations, and then calculate the temperature and
density dependence of the basin energy, degeneracy, and shape. The
temperature dependence of the energy of the minima is qualitatively
similar to simple liquids, but has anomalous density dependence. The
unusual density dependence is also reflected in the configurational
entropy, the thermodynamic measure of degeneracy. Finally, we study the
structure of simulated water at the minima, which provides insight on
the progressive tetrahedral ordering of the liquid on cooling.
Starr, Francis W.; Sastry, Srikanth; La Nave, Emilia; Scala, Antonio; Stanley, H. Eugene; Sciortino, F
Thermodynamic and structural aspects of the potential energy surface of simulated water Journal Article
In: PHYSICAL REVIEW E, vol. 63, no. 4, 1, pp. 041201, 2001, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{sslsss01,
title = {Thermodynamic and structural aspects of the potential energy surface of simulated water},
author = {Starr, Francis W. and Sastry, Srikanth and La Nave, Emilia and Scala, Antonio and Stanley, H. Eugene and Sciortino, F},
url = {http://fstarr.web.wesleyan.edu/publications/sslsss.pdf},
doi = {10.1103/PhysRevE.63.041201},
issn = {1063-651X},
year = {2001},
date = {2001-04-01},
journal = {PHYSICAL REVIEW E},
volume = {63},
number = {4, 1},
pages = {041201},
abstract = {Relations between the thermodynamics and dynamics of supercooled liquids approaching a glass transition is a topic of considerable interest. The potential energy surface of model liquids has been increasingly studied, since it provides a connection between the configurational component of the partition function on the one hand, and the system dynamics on the other. This connection is most obvious at low temperatures, where the motion of the system can be partitioned into vibrations within a basin of attraction and infrequent interbasin transitions. in this work, we present a description of the potential energy surface properties of supercooled liquid water. The dynamics of this model have been studied in great detail in recent years. We locate the minima sampled by the liquid by ``quenches'' from equilibrium configurations generated via molecular dynamics simulations, and then calculate the temperature and density dependence of the basin energy, degeneracy, and shape. The temperature dependence of the energy of the minima is qualitatively similar to simple liquids, but has anomalous density dependence. The unusual density dependence is also reflected in the configurational entropy, the thermodynamic measure of degeneracy. Finally, we study the structure of simulated water at the minima, which provides insight on the progressive tetrahedral ordering of the liquid on cooling.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Relations between the thermodynamics and dynamics of supercooled liquids approaching a glass transition is a topic of considerable interest. The potential energy surface of model liquids has been increasingly studied, since it provides a connection between the configurational component of the partition function on the one hand, and the system dynamics on the other. This connection is most obvious at low temperatures, where the motion of the system can be partitioned into vibrations within a basin of attraction and infrequent interbasin transitions. in this work, we present a description of the potential energy surface properties of supercooled liquid water. The dynamics of this model have been studied in great detail in recent years. We locate the minima sampled by the liquid by ``quenches'' from equilibrium configurations generated via molecular dynamics simulations, and then calculate the temperature and density dependence of the basin energy, degeneracy, and shape. The temperature dependence of the energy of the minima is qualitatively similar to simple liquids, but has anomalous density dependence. The unusual density dependence is also reflected in the configurational entropy, the thermodynamic measure of degeneracy. Finally, we study the structure of simulated water at the minima, which provides insight on the progressive tetrahedral ordering of the liquid on cooling.
2000
Scala, Antonio; Starr, Francis W; Nave, Emilia La; Stanley, Eugene H; Sciortino, Francesco
Free energy surface of supercooled water Journal Article
In: PHYSICAL REVIEW E, vol. 62, no. 6, A, pp. 8016-8020, 2000, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{sslss-preb,
title = {Free energy surface of supercooled water},
author = {Antonio Scala and Francis W Starr and Emilia La Nave and Eugene H Stanley and Francesco Sciortino},
url = {http://fstarr.web.wesleyan.edu/publications/sslss-pre.pdf},
doi = {10.1103/PhysRevE.62.8016},
issn = {1063-651X},
year = {2000},
date = {2000-12-01},
journal = {PHYSICAL REVIEW E},
volume = {62},
number = {6, A},
pages = {8016-8020},
abstract = {We present a detailed analysis of the free energy surface of a well
characterized rigid model for water in supercooled states. We propose a
functional form for the liquid free energy, supported by recent
theoretical predictions [Y. Rosenfeld and P. Tarazona, Mel. Phys. 95,
141 (1998)], and use it to locate the position of a liquid-liquid critical point at T-C' = 130+/-5 K, P-C' = 290+/-30 MPa, and rho (C') =
1.10+/-0.03 g/cm(3). The observation of the critical point strengthens
the possibility that the extended simple point charge model of water may
undergo a liquid-liquid phase transition. Finally, we discuss the
possibility that the approach to the liquid-liquid critical point could
be pre-empted by the glass transition.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We present a detailed analysis of the free energy surface of a well
characterized rigid model for water in supercooled states. We propose a
functional form for the liquid free energy, supported by recent
theoretical predictions [Y. Rosenfeld and P. Tarazona, Mel. Phys. 95,
141 (1998)], and use it to locate the position of a liquid-liquid critical point at T-C' = 130+/-5 K, P-C' = 290+/-30 MPa, and rho (C') =
1.10+/-0.03 g/cm(3). The observation of the critical point strengthens
the possibility that the extended simple point charge model of water may
undergo a liquid-liquid phase transition. Finally, we discuss the
possibility that the approach to the liquid-liquid critical point could
be pre-empted by the glass transition.
characterized rigid model for water in supercooled states. We propose a
functional form for the liquid free energy, supported by recent
theoretical predictions [Y. Rosenfeld and P. Tarazona, Mel. Phys. 95,
141 (1998)], and use it to locate the position of a liquid-liquid critical point at T-C' = 130+/-5 K, P-C' = 290+/-30 MPa, and rho (C') =
1.10+/-0.03 g/cm(3). The observation of the critical point strengthens
the possibility that the extended simple point charge model of water may
undergo a liquid-liquid phase transition. Finally, we discuss the
possibility that the approach to the liquid-liquid critical point could
be pre-empted by the glass transition.
Scala, Antonio; Starr, Francis W.; La Nave, Emilia; Stanley, H. Eugene; Sciortino, Francesco
Free energy surface of supercooled water Journal Article
In: PHYSICAL REVIEW E, vol. 62, no. 6, A, pp. 8016-8020, 2000, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{sslss-pre,
title = {Free energy surface of supercooled water},
author = {Scala, Antonio and Starr, Francis W. and La Nave, Emilia and Stanley, H. Eugene and Sciortino, Francesco},
url = {http://fstarr.web.wesleyan.edu/publications/sslss-pre.pdf},
doi = {10.1103/PhysRevE.62.8016},
issn = {1063-651X},
year = {2000},
date = {2000-12-01},
journal = {PHYSICAL REVIEW E},
volume = {62},
number = {6, A},
pages = {8016-8020},
abstract = {We present a detailed analysis of the free energy surface of a well characterized rigid model for water in supercooled states. We propose a functional form for the liquid free energy, supported by recent theoretical predictions [Y. Rosenfeld and P. Tarazona, Mel. Phys. 95, 141 (1998)], and use it to locate the position of a liquid-liquid critical point at T-C' = 130+/-5 K, P-C' = 290+/-30 MPa, and rho (C') = 1.10+/-0.03 g/cm(3). The observation of the critical point strengthens the possibility that the extended simple point charge model of water may undergo a liquid-liquid phase transition. Finally, we discuss the possibility that the approach to the liquid-liquid critical point could be pre-empted by the glass transition.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We present a detailed analysis of the free energy surface of a well characterized rigid model for water in supercooled states. We propose a functional form for the liquid free energy, supported by recent theoretical predictions [Y. Rosenfeld and P. Tarazona, Mel. Phys. 95, 141 (1998)], and use it to locate the position of a liquid-liquid critical point at T-C' = 130+/-5 K, P-C' = 290+/-30 MPa, and rho (C') = 1.10+/-0.03 g/cm(3). The observation of the critical point strengthens the possibility that the extended simple point charge model of water may undergo a liquid-liquid phase transition. Finally, we discuss the possibility that the approach to the liquid-liquid critical point could be pre-empted by the glass transition.
Scala, Antonio; Starr, Francis W; Nave, Emilia La; Sciortino, Francesco; Stanley, Eugene H
Configurational entropy and diffusivity of supercooled water Journal Article
In: NATURE, vol. 406, no. 6792, pp. 166-169, 2000, ISSN: 0028-0836.
Abstract | BibTeX | Tags: | Links:
@article{sslss-natureb,
title = {Configurational entropy and diffusivity of supercooled water},
author = {Antonio Scala and Francis W Starr and Emilia La Nave and Francesco Sciortino and Eugene H Stanley},
url = {http://fstarr.web.wesleyan.edu/publications/sslss-nature.pdf},
issn = {0028-0836},
year = {2000},
date = {2000-07-01},
journal = {NATURE},
volume = {406},
number = {6792},
pages = {166-169},
abstract = {As a liquid approaches the glass transition, its properties are
dominated by local potential minima(1,2) in its energy landscape. The
liquid experiences localized vibrations in the basins of attraction
surrounding the minima, and rearranges via relatively infrequent
inter-basin jumps(3). As a result, the liquid dynamics at low
temperature are related to the system's exploration of its own
configuration space. The `thermodynamic approach' to the glass
transition considers the reduction in configuration space(4-8) explored
as the system cools, and predicts that the configurational
entropy(5,9,10) (a measure of the number of local potential energy
minima sampled by the liquid) is related to the diffusion constant. Here
we report a stringent test of the thermodynamic approach for liquid
water (a convenient system to study because of an anomalous pressure
dependence in the diffusion constant). We calculate the configurational
entropy at points spanning a large region of the temperature-density
plane, using a model(11) that reproduces the dynamical anomalies of
liquid water. We find that the thermodynamic approach can be used to
understand the characteristic dynamic anomalies, and that the diffusive
dynamics are governed by the configurational entropy. Our results
indicate that the thermodynamic approach might be extended to predict
the dynamical behaviour of supercooled liquids in general.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
As a liquid approaches the glass transition, its properties are
dominated by local potential minima(1,2) in its energy landscape. The
liquid experiences localized vibrations in the basins of attraction
surrounding the minima, and rearranges via relatively infrequent
inter-basin jumps(3). As a result, the liquid dynamics at low
temperature are related to the system's exploration of its own
configuration space. The `thermodynamic approach' to the glass
transition considers the reduction in configuration space(4-8) explored
as the system cools, and predicts that the configurational
entropy(5,9,10) (a measure of the number of local potential energy
minima sampled by the liquid) is related to the diffusion constant. Here
we report a stringent test of the thermodynamic approach for liquid
water (a convenient system to study because of an anomalous pressure
dependence in the diffusion constant). We calculate the configurational
entropy at points spanning a large region of the temperature-density
plane, using a model(11) that reproduces the dynamical anomalies of
liquid water. We find that the thermodynamic approach can be used to
understand the characteristic dynamic anomalies, and that the diffusive
dynamics are governed by the configurational entropy. Our results
indicate that the thermodynamic approach might be extended to predict
the dynamical behaviour of supercooled liquids in general.
dominated by local potential minima(1,2) in its energy landscape. The
liquid experiences localized vibrations in the basins of attraction
surrounding the minima, and rearranges via relatively infrequent
inter-basin jumps(3). As a result, the liquid dynamics at low
temperature are related to the system's exploration of its own
configuration space. The `thermodynamic approach' to the glass
transition considers the reduction in configuration space(4-8) explored
as the system cools, and predicts that the configurational
entropy(5,9,10) (a measure of the number of local potential energy
minima sampled by the liquid) is related to the diffusion constant. Here
we report a stringent test of the thermodynamic approach for liquid
water (a convenient system to study because of an anomalous pressure
dependence in the diffusion constant). We calculate the configurational
entropy at points spanning a large region of the temperature-density
plane, using a model(11) that reproduces the dynamical anomalies of
liquid water. We find that the thermodynamic approach can be used to
understand the characteristic dynamic anomalies, and that the diffusive
dynamics are governed by the configurational entropy. Our results
indicate that the thermodynamic approach might be extended to predict
the dynamical behaviour of supercooled liquids in general.
Starr, Francis W; Nielsen, Johannes K; Stanley, Eugene H
Hydrogen-bond dynamics for the extended simple point-charge model of water Journal Article
In: PHYSICAL REVIEW E, vol. 62, no. 1, A, pp. 579-587, 2000, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{sns-preb,
title = {Hydrogen-bond dynamics for the extended simple point-charge model of
water},
author = {Francis W Starr and Johannes K Nielsen and Eugene H Stanley},
url = {http://fstarr.web.wesleyan.edu/publications/sns-pre},
doi = {10.1103/PhysRevE.62.579},
issn = {1063-651X},
year = {2000},
date = {2000-07-01},
journal = {PHYSICAL REVIEW E},
volume = {62},
number = {1, A},
pages = {579-587},
abstract = {We study hydrogen-bond dynamics in liquid water at low temperatures
using molecular dynamics simulations. We analyze the dynamics using
energetic and geometric definitions of a hydrogen bond, and employ two
analysis methods: (i) a history-dependent correlation function, related
to the distribution of bond lifetimes, and (ii) a history-independent
correlation function. For method (i) we find an approximately Arrhenius
temperature dependence of the bond lifetime, and find that the
distribution of bond lifetimes is extremely sensitive to the choice of
bond definition. For method (ii) we find-independent of bond
definition-that the dynamics are consistent with the predictions of the
mode-coupling theory, suggesting that the slow dynamics of hydrogen
bonds can be explained in the same framework as standard transport
quantities. Our results allow us to clarify the significance of the
choice of both bond definition and analysis technique.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We study hydrogen-bond dynamics in liquid water at low temperatures
using molecular dynamics simulations. We analyze the dynamics using
energetic and geometric definitions of a hydrogen bond, and employ two
analysis methods: (i) a history-dependent correlation function, related
to the distribution of bond lifetimes, and (ii) a history-independent
correlation function. For method (i) we find an approximately Arrhenius
temperature dependence of the bond lifetime, and find that the
distribution of bond lifetimes is extremely sensitive to the choice of
bond definition. For method (ii) we find-independent of bond
definition-that the dynamics are consistent with the predictions of the
mode-coupling theory, suggesting that the slow dynamics of hydrogen
bonds can be explained in the same framework as standard transport
quantities. Our results allow us to clarify the significance of the
choice of both bond definition and analysis technique.
using molecular dynamics simulations. We analyze the dynamics using
energetic and geometric definitions of a hydrogen bond, and employ two
analysis methods: (i) a history-dependent correlation function, related
to the distribution of bond lifetimes, and (ii) a history-independent
correlation function. For method (i) we find an approximately Arrhenius
temperature dependence of the bond lifetime, and find that the
distribution of bond lifetimes is extremely sensitive to the choice of
bond definition. For method (ii) we find-independent of bond
definition-that the dynamics are consistent with the predictions of the
mode-coupling theory, suggesting that the slow dynamics of hydrogen
bonds can be explained in the same framework as standard transport
quantities. Our results allow us to clarify the significance of the
choice of both bond definition and analysis technique.
Scala, Antonio; Starr, Francis W.; La Nave, Emilia; Sciortino, Francesco; Stanley, H. Eugene
Configurational entropy and diffusivity of supercooled water Journal Article
In: NATURE, vol. 406, no. 6792, pp. 166-169, 2000, ISSN: 0028-0836.
Abstract | BibTeX | Tags: Glass Formation, Water | Links:
@article{sslss-nature,
title = {Configurational entropy and diffusivity of supercooled water},
author = {Scala, Antonio and Starr, Francis W. and La Nave, Emilia and Sciortino, Francesco and Stanley, H. Eugene},
url = {http://fstarr.web.wesleyan.edu/publications/sslss-nature.pdf},
issn = {0028-0836},
year = {2000},
date = {2000-07-01},
journal = {NATURE},
volume = {406},
number = {6792},
pages = {166-169},
abstract = {As a liquid approaches the glass transition, its properties are dominated by local potential minima(1,2) in its energy landscape. The liquid experiences localized vibrations in the basins of attraction surrounding the minima, and rearranges via relatively infrequent inter-basin jumps(3). As a result, the liquid dynamics at low temperature are related to the system's exploration of its own configuration space. The `thermodynamic approach' to the glass transition considers the reduction in configuration space(4-8) explored as the system cools, and predicts that the configurational entropy(5,9,10) (a measure of the number of local potential energy minima sampled by the liquid) is related to the diffusion constant. Here we report a stringent test of the thermodynamic approach for liquid water (a convenient system to study because of an anomalous pressure dependence in the diffusion constant). We calculate the configurational entropy at points spanning a large region of the temperature-density plane, using a model(11) that reproduces the dynamical anomalies of liquid water. We find that the thermodynamic approach can be used to understand the characteristic dynamic anomalies, and that the diffusive dynamics are governed by the configurational entropy. Our results indicate that the thermodynamic approach might be extended to predict the dynamical behaviour of supercooled liquids in general.},
keywords = {Glass Formation, Water},
pubstate = {published},
tppubtype = {article}
}
As a liquid approaches the glass transition, its properties are dominated by local potential minima(1,2) in its energy landscape. The liquid experiences localized vibrations in the basins of attraction surrounding the minima, and rearranges via relatively infrequent inter-basin jumps(3). As a result, the liquid dynamics at low temperature are related to the system's exploration of its own configuration space. The `thermodynamic approach' to the glass transition considers the reduction in configuration space(4-8) explored as the system cools, and predicts that the configurational entropy(5,9,10) (a measure of the number of local potential energy minima sampled by the liquid) is related to the diffusion constant. Here we report a stringent test of the thermodynamic approach for liquid water (a convenient system to study because of an anomalous pressure dependence in the diffusion constant). We calculate the configurational entropy at points spanning a large region of the temperature-density plane, using a model(11) that reproduces the dynamical anomalies of liquid water. We find that the thermodynamic approach can be used to understand the characteristic dynamic anomalies, and that the diffusive dynamics are governed by the configurational entropy. Our results indicate that the thermodynamic approach might be extended to predict the dynamical behaviour of supercooled liquids in general.
Starr, Francis W.; Nielsen, Johannes K.; Stanley, H. Eugene
Hydrogen-bond dynamics for the extended simple point-charge model of water Journal Article
In: PHYSICAL REVIEW E, vol. 62, no. 1, A, pp. 579-587, 2000, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{sns-pre,
title = {Hydrogen-bond dynamics for the extended simple point-charge model of water},
author = {Starr, Francis W. and Nielsen, Johannes K. and Stanley, H. Eugene},
url = {http://fstarr.web.wesleyan.edu/publications/sns-pre},
doi = {10.1103/PhysRevE.62.579},
issn = {1063-651X},
year = {2000},
date = {2000-07-01},
journal = {PHYSICAL REVIEW E},
volume = {62},
number = {1, A},
pages = {579-587},
abstract = {We study hydrogen-bond dynamics in liquid water at low temperatures using molecular dynamics simulations. We analyze the dynamics using energetic and geometric definitions of a hydrogen bond, and employ two analysis methods: (i) a history-dependent correlation function, related to the distribution of bond lifetimes, and (ii) a history-independent correlation function. For method (i) we find an approximately Arrhenius temperature dependence of the bond lifetime, and find that the distribution of bond lifetimes is extremely sensitive to the choice of bond definition. For method (ii) we find-independent of bond definition-that the dynamics are consistent with the predictions of the mode-coupling theory, suggesting that the slow dynamics of hydrogen bonds can be explained in the same framework as standard transport quantities. Our results allow us to clarify the significance of the choice of both bond definition and analysis technique.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We study hydrogen-bond dynamics in liquid water at low temperatures using molecular dynamics simulations. We analyze the dynamics using energetic and geometric definitions of a hydrogen bond, and employ two analysis methods: (i) a history-dependent correlation function, related to the distribution of bond lifetimes, and (ii) a history-independent correlation function. For method (i) we find an approximately Arrhenius temperature dependence of the bond lifetime, and find that the distribution of bond lifetimes is extremely sensitive to the choice of bond definition. For method (ii) we find-independent of bond definition-that the dynamics are consistent with the predictions of the mode-coupling theory, suggesting that the slow dynamics of hydrogen bonds can be explained in the same framework as standard transport quantities. Our results allow us to clarify the significance of the choice of both bond definition and analysis technique.
Nave, Emilia La; Scala, Antonio; Starr, Francis W; Sciortino, Francesco; Stanley, Eugene H
Instantaneous normal mode analysis of supercooled water Journal Article
In: PHYSICAL REVIEW LETTERS, vol. 84, no. 20, pp. 4605-4608, 2000, ISSN: 0031-9007.
Abstract | BibTeX | Tags: | Links:
@article{lssss00b,
title = {Instantaneous normal mode analysis of supercooled water},
author = {Emilia La Nave and Antonio Scala and Francis W Starr and Francesco Sciortino and Eugene H Stanley},
url = {http://fstarr.web.wesleyan.edu/publications/lssss.pdf},
doi = {10.1103/PhysRevLett.84.4605},
issn = {0031-9007},
year = {2000},
date = {2000-05-01},
journal = {PHYSICAL REVIEW LETTERS},
volume = {84},
number = {20},
pages = {4605-4608},
abstract = {We use the instantaneous normal mode approach to provide a description
of the local curvature of the potential energy surface of a model for
water. We focus on the region of the phase diagram in which the dynamics
may be described by mode-coupling theory. We find that the diffusion
constant depends on the fraction of directions in configuration space
connecting different local minima, supporting the hypothesis that the
dynamics are controlled by the geometric properties of configuration
space. Furthermore, we find a relation between the number of basins
accessed in equilibrium and the connectivity between them.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We use the instantaneous normal mode approach to provide a description
of the local curvature of the potential energy surface of a model for
water. We focus on the region of the phase diagram in which the dynamics
may be described by mode-coupling theory. We find that the diffusion
constant depends on the fraction of directions in configuration space
connecting different local minima, supporting the hypothesis that the
dynamics are controlled by the geometric properties of configuration
space. Furthermore, we find a relation between the number of basins
accessed in equilibrium and the connectivity between them.
of the local curvature of the potential energy surface of a model for
water. We focus on the region of the phase diagram in which the dynamics
may be described by mode-coupling theory. We find that the diffusion
constant depends on the fraction of directions in configuration space
connecting different local minima, supporting the hypothesis that the
dynamics are controlled by the geometric properties of configuration
space. Furthermore, we find a relation between the number of basins
accessed in equilibrium and the connectivity between them.
La Nave, Emilia; Scala, Antonio; Starr, Francis W.; Sciortino, Francesco; Stanley, H. Eugene
Instantaneous normal mode analysis of supercooled water Journal Article
In: PHYSICAL REVIEW LETTERS, vol. 84, no. 20, pp. 4605-4608, 2000, ISSN: 0031-9007.
Abstract | BibTeX | Tags: | Links:
@article{lssss00,
title = {Instantaneous normal mode analysis of supercooled water},
author = {La Nave, Emilia and Scala, Antonio and Starr, Francis W. and Sciortino, Francesco and Stanley, H. Eugene},
url = {http://fstarr.web.wesleyan.edu/publications/lssss.pdf},
doi = {10.1103/PhysRevLett.84.4605},
issn = {0031-9007},
year = {2000},
date = {2000-05-01},
journal = {PHYSICAL REVIEW LETTERS},
volume = {84},
number = {20},
pages = {4605-4608},
abstract = {We use the instantaneous normal mode approach to provide a description of the local curvature of the potential energy surface of a model for water. We focus on the region of the phase diagram in which the dynamics may be described by mode-coupling theory. We find that the diffusion constant depends on the fraction of directions in configuration space connecting different local minima, supporting the hypothesis that the dynamics are controlled by the geometric properties of configuration space. Furthermore, we find a relation between the number of basins accessed in equilibrium and the connectivity between them.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We use the instantaneous normal mode approach to provide a description of the local curvature of the potential energy surface of a model for water. We focus on the region of the phase diagram in which the dynamics may be described by mode-coupling theory. We find that the diffusion constant depends on the fraction of directions in configuration space connecting different local minima, supporting the hypothesis that the dynamics are controlled by the geometric properties of configuration space. Furthermore, we find a relation between the number of basins accessed in equilibrium and the connectivity between them.
Stanley, Eugene H; Buldyrev, Sergey V; Canpolat, Murat; Mishima, Osamu; Sadr-Lahijany, MR; Scala, Antonio; Starr, Francis W
The puzzling behavior of water at very low temperature Journal Article
In: PHYSICAL CHEMISTRY CHEMICAL PHYSICS, vol. 2, no. 8, pp. 1551-1558, 2000, ISSN: 1463-9076.
Abstract | BibTeX | Tags: | Links:
@article{dortmund00b,
title = {The puzzling behavior of water at very low temperature},
author = {Eugene H Stanley and Sergey V Buldyrev and Murat Canpolat and Osamu Mishima and MR Sadr-Lahijany and Antonio Scala and Francis W Starr},
url = {http://fstarr.web.wesleyan.edu/publications/dortmund.pdf},
doi = {10.1039/b000058m},
issn = {1463-9076},
year = {2000},
date = {2000-01-01},
journal = {PHYSICAL CHEMISTRY CHEMICAL PHYSICS},
volume = {2},
number = {8},
pages = {1551-1558},
abstract = {Although H2O has been the topic of considerable research since the
beginning of the century, most of its anomalous physical properties are
still not well understood. First we discuss some of the anomalies of
this ``complex fluid.'' Then we describe a qualitative interpretation in
terms of percolation concepts. Finally, we discuss recent experiments
and simulations relating to the liquid-liquid phase transition
hypothesis that, in addition to the known critical point in water, there
may exist a ``second'' critical point at low temperatures. In
particular, we discuss very recent measurements at Tsukuba of the
compression-induced melting and decompression-induced melting lines of
high-pressure forms of ice. We show how knowledge of these lines enables
one to obtain an approximation for the Gibbs potential G(P,T) and the
equation of state V(P,T) for water, both of which are consistent with
the possible continuity of liquid water and the amorphous forms of solid
water.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Although H2O has been the topic of considerable research since the
beginning of the century, most of its anomalous physical properties are
still not well understood. First we discuss some of the anomalies of
this ``complex fluid.'' Then we describe a qualitative interpretation in
terms of percolation concepts. Finally, we discuss recent experiments
and simulations relating to the liquid-liquid phase transition
hypothesis that, in addition to the known critical point in water, there
may exist a ``second'' critical point at low temperatures. In
particular, we discuss very recent measurements at Tsukuba of the
compression-induced melting and decompression-induced melting lines of
high-pressure forms of ice. We show how knowledge of these lines enables
one to obtain an approximation for the Gibbs potential G(P,T) and the
equation of state V(P,T) for water, both of which are consistent with
the possible continuity of liquid water and the amorphous forms of solid
water.
beginning of the century, most of its anomalous physical properties are
still not well understood. First we discuss some of the anomalies of
this ``complex fluid.'' Then we describe a qualitative interpretation in
terms of percolation concepts. Finally, we discuss recent experiments
and simulations relating to the liquid-liquid phase transition
hypothesis that, in addition to the known critical point in water, there
may exist a ``second'' critical point at low temperatures. In
particular, we discuss very recent measurements at Tsukuba of the
compression-induced melting and decompression-induced melting lines of
high-pressure forms of ice. We show how knowledge of these lines enables
one to obtain an approximation for the Gibbs potential G(P,T) and the
equation of state V(P,T) for water, both of which are consistent with
the possible continuity of liquid water and the amorphous forms of solid
water.
Stanley, H. Eugene; Buldyrev, Sergey V.; Canpolat, Murat; Mishima, Osamu; Sadr-Lahijany, MR; Scala, Antonio; Starr, Francis W.
The puzzling behavior of water at very low temperature Journal Article
In: PHYSICAL CHEMISTRY CHEMICAL PHYSICS, vol. 2, no. 8, pp. 1551-1558, 2000, ISSN: 1463-9076.
Abstract | BibTeX | Tags: | Links:
@article{dortmund00,
title = {The puzzling behavior of water at very low temperature},
author = {Stanley, H. Eugene and Buldyrev, Sergey V. and Canpolat, Murat and Mishima, Osamu and Sadr-Lahijany, MR and Scala, Antonio and Starr, Francis W.},
url = {http://fstarr.web.wesleyan.edu/publications/dortmund.pdf},
doi = {10.1039/b000058m},
issn = {1463-9076},
year = {2000},
date = {2000-01-01},
journal = {PHYSICAL CHEMISTRY CHEMICAL PHYSICS},
volume = {2},
number = {8},
pages = {1551-1558},
abstract = {Although H2O has been the topic of considerable research since the beginning of the century, most of its anomalous physical properties are still not well understood. First we discuss some of the anomalies of this ``complex fluid.'' Then we describe a qualitative interpretation in terms of percolation concepts. Finally, we discuss recent experiments and simulations relating to the liquid-liquid phase transition hypothesis that, in addition to the known critical point in water, there may exist a ``second'' critical point at low temperatures. In particular, we discuss very recent measurements at Tsukuba of the compression-induced melting and decompression-induced melting lines of high-pressure forms of ice. We show how knowledge of these lines enables one to obtain an approximation for the Gibbs potential G(P,T) and the equation of state V(P,T) for water, both of which are consistent with the possible continuity of liquid water and the amorphous forms of solid water.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Although H2O has been the topic of considerable research since the beginning of the century, most of its anomalous physical properties are still not well understood. First we discuss some of the anomalies of this ``complex fluid.'' Then we describe a qualitative interpretation in terms of percolation concepts. Finally, we discuss recent experiments and simulations relating to the liquid-liquid phase transition hypothesis that, in addition to the known critical point in water, there may exist a ``second'' critical point at low temperatures. In particular, we discuss very recent measurements at Tsukuba of the compression-induced melting and decompression-induced melting lines of high-pressure forms of ice. We show how knowledge of these lines enables one to obtain an approximation for the Gibbs potential G(P,T) and the equation of state V(P,T) for water, both of which are consistent with the possible continuity of liquid water and the amorphous forms of solid water.
1999
Starr, Francis W; Sciortino, Francesco; Stanley, Eugene H
Dynamics of simulated water under pressure Journal Article
In: PHYSICAL REVIEW E, vol. 60, no. 6, A, pp. 6757-6768, 1999, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{sss99b,
title = {Dynamics of simulated water under pressure},
author = {Francis W Starr and Francesco Sciortino and Eugene H Stanley},
url = {http://fstarr.web.wesleyan.edu/publications/sss.pdf},
doi = {10.1103/PhysRevE.60.6757},
issn = {1063-651X},
year = {1999},
date = {1999-12-01},
journal = {PHYSICAL REVIEW E},
volume = {60},
number = {6, A},
pages = {6757-6768},
abstract = {We present molecular dynamics simulations of the extended
simple-point-charge model of water to probe the dynamic properties at
temperatures from 350 K down to 190 K and pressures from 2.5 GPa (25
kbar) down to -300 MPa (-3 kbar). We compare our results with those
obtained experimentally, both of which show a diffusivity maximum as a
function of pressure. We find that our simulation results are consistent
with the predictions of the mode-coupling theory for the dynamics of
weakly supercooled liquids-strongly supporting the hypothesis that the
apparent divergences of dynamic properties observed experimentally may
be independent of a possible thermodynamic singularity at low
temperature. The dramatic change in water's dynamic and structural
properties as a function of pressure allows us to confirm the
predictions of MCT over a much broader range of the von Schweidler
exponent values than has been studied for simple atomic liquids. We also
show how structural changes are reflected in the wave-vector dependence
of dynamic properties of the liquid along a path of nearly constant
diffusivity. For temperatures below the crossover temperature of MCT
(where the predictions of MCT are expected to fail), we find tentative
evidence for a crossover of the temperature dependence of the
diffusivity from power-law to Arrhenius behavior, with an activation
energy typical of a strong liquid. [S1063-651X(99)11712-4].},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We present molecular dynamics simulations of the extended
simple-point-charge model of water to probe the dynamic properties at
temperatures from 350 K down to 190 K and pressures from 2.5 GPa (25
kbar) down to -300 MPa (-3 kbar). We compare our results with those
obtained experimentally, both of which show a diffusivity maximum as a
function of pressure. We find that our simulation results are consistent
with the predictions of the mode-coupling theory for the dynamics of
weakly supercooled liquids-strongly supporting the hypothesis that the
apparent divergences of dynamic properties observed experimentally may
be independent of a possible thermodynamic singularity at low
temperature. The dramatic change in water's dynamic and structural
properties as a function of pressure allows us to confirm the
predictions of MCT over a much broader range of the von Schweidler
exponent values than has been studied for simple atomic liquids. We also
show how structural changes are reflected in the wave-vector dependence
of dynamic properties of the liquid along a path of nearly constant
diffusivity. For temperatures below the crossover temperature of MCT
(where the predictions of MCT are expected to fail), we find tentative
evidence for a crossover of the temperature dependence of the
diffusivity from power-law to Arrhenius behavior, with an activation
energy typical of a strong liquid. [S1063-651X(99)11712-4].
simple-point-charge model of water to probe the dynamic properties at
temperatures from 350 K down to 190 K and pressures from 2.5 GPa (25
kbar) down to -300 MPa (-3 kbar). We compare our results with those
obtained experimentally, both of which show a diffusivity maximum as a
function of pressure. We find that our simulation results are consistent
with the predictions of the mode-coupling theory for the dynamics of
weakly supercooled liquids-strongly supporting the hypothesis that the
apparent divergences of dynamic properties observed experimentally may
be independent of a possible thermodynamic singularity at low
temperature. The dramatic change in water's dynamic and structural
properties as a function of pressure allows us to confirm the
predictions of MCT over a much broader range of the von Schweidler
exponent values than has been studied for simple atomic liquids. We also
show how structural changes are reflected in the wave-vector dependence
of dynamic properties of the liquid along a path of nearly constant
diffusivity. For temperatures below the crossover temperature of MCT
(where the predictions of MCT are expected to fail), we find tentative
evidence for a crossover of the temperature dependence of the
diffusivity from power-law to Arrhenius behavior, with an activation
energy typical of a strong liquid. [S1063-651X(99)11712-4].
Starr, Francis W.; Sciortino, Francesco; Stanley, H. Eugene
Dynamics of simulated water under pressure Journal Article
In: PHYSICAL REVIEW E, vol. 60, no. 6, A, pp. 6757-6768, 1999, ISSN: 1063-651X.
Abstract | BibTeX | Tags: Glass Formation, Water | Links:
@article{sss99,
title = {Dynamics of simulated water under pressure},
author = {Starr, Francis W. and Sciortino, Francesco and Stanley, H. Eugene},
url = {http://fstarr.web.wesleyan.edu/publications/sss.pdf},
doi = {10.1103/PhysRevE.60.6757},
issn = {1063-651X},
year = {1999},
date = {1999-12-01},
journal = {PHYSICAL REVIEW E},
volume = {60},
number = {6, A},
pages = {6757-6768},
abstract = {We present molecular dynamics simulations of the extended simple-point-charge model of water to probe the dynamic properties at temperatures from 350 K down to 190 K and pressures from 2.5 GPa (25 kbar) down to -300 MPa (-3 kbar). We compare our results with those obtained experimentally, both of which show a diffusivity maximum as a function of pressure. We find that our simulation results are consistent with the predictions of the mode-coupling theory for the dynamics of weakly supercooled liquids-strongly supporting the hypothesis that the apparent divergences of dynamic properties observed experimentally may be independent of a possible thermodynamic singularity at low temperature. The dramatic change in water's dynamic and structural properties as a function of pressure allows us to confirm the predictions of MCT over a much broader range of the von Schweidler exponent values than has been studied for simple atomic liquids. We also show how structural changes are reflected in the wave-vector dependence of dynamic properties of the liquid along a path of nearly constant diffusivity. For temperatures below the crossover temperature of MCT (where the predictions of MCT are expected to fail), we find tentative evidence for a crossover of the temperature dependence of the diffusivity from power-law to Arrhenius behavior, with an activation energy typical of a strong liquid. [S1063-651X(99)11712-4].},
keywords = {Glass Formation, Water},
pubstate = {published},
tppubtype = {article}
}
We present molecular dynamics simulations of the extended simple-point-charge model of water to probe the dynamic properties at temperatures from 350 K down to 190 K and pressures from 2.5 GPa (25 kbar) down to -300 MPa (-3 kbar). We compare our results with those obtained experimentally, both of which show a diffusivity maximum as a function of pressure. We find that our simulation results are consistent with the predictions of the mode-coupling theory for the dynamics of weakly supercooled liquids-strongly supporting the hypothesis that the apparent divergences of dynamic properties observed experimentally may be independent of a possible thermodynamic singularity at low temperature. The dramatic change in water's dynamic and structural properties as a function of pressure allows us to confirm the predictions of MCT over a much broader range of the von Schweidler exponent values than has been studied for simple atomic liquids. We also show how structural changes are reflected in the wave-vector dependence of dynamic properties of the liquid along a path of nearly constant diffusivity. For temperatures below the crossover temperature of MCT (where the predictions of MCT are expected to fail), we find tentative evidence for a crossover of the temperature dependence of the diffusivity from power-law to Arrhenius behavior, with an activation energy typical of a strong liquid. [S1063-651X(99)11712-4].
Starr, Francis W; Bellissent-Funel, Mairie Claire; Stanley, Eugene H
Structure of supercooled and glassy water under pressure Journal Article
In: PHYSICAL REVIEW E, vol. 60, no. 1, pp. 1084-1087, 1999, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{sbs99b,
title = {Structure of supercooled and glassy water under pressure},
author = {Francis W Starr and Mairie Claire Bellissent-Funel and Eugene H Stanley},
url = {http://fstarr.web.wesleyan.edu/publications/sbs.pdf},
doi = {10.1103/PhysRevE.60.1084},
issn = {1063-651X},
year = {1999},
date = {1999-07-01},
journal = {PHYSICAL REVIEW E},
volume = {60},
number = {1},
pages = {1084-1087},
abstract = {We use molecular-dynamics simulations to study the effect of temperature
and pressure on the local structure of liquid water in parallel with
neutron-scattering experiments. We find, in agreement with experimental
results, that the simulated liquid structure at high pressure is nearly
independent of temperature, and remarkably similar to the known
structure of the high-density amorphous ice. Further, at low pressure,
the liquid structure appears to approach the experimentally measured
structure of low-density amorphous ice as temperature decreases. These
results are consistent with the postulated continuity between the liquid
and glassy phases of H2O. [S1063-651X(99)10007-2].},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We use molecular-dynamics simulations to study the effect of temperature
and pressure on the local structure of liquid water in parallel with
neutron-scattering experiments. We find, in agreement with experimental
results, that the simulated liquid structure at high pressure is nearly
independent of temperature, and remarkably similar to the known
structure of the high-density amorphous ice. Further, at low pressure,
the liquid structure appears to approach the experimentally measured
structure of low-density amorphous ice as temperature decreases. These
results are consistent with the postulated continuity between the liquid
and glassy phases of H2O. [S1063-651X(99)10007-2].
and pressure on the local structure of liquid water in parallel with
neutron-scattering experiments. We find, in agreement with experimental
results, that the simulated liquid structure at high pressure is nearly
independent of temperature, and remarkably similar to the known
structure of the high-density amorphous ice. Further, at low pressure,
the liquid structure appears to approach the experimentally measured
structure of low-density amorphous ice as temperature decreases. These
results are consistent with the postulated continuity between the liquid
and glassy phases of H2O. [S1063-651X(99)10007-2].
Starr, Francis W.; Bellissent-Funel, Mairie Claire; Stanley, H. Eugene
Structure of supercooled and glassy water under pressure Journal Article
In: PHYSICAL REVIEW E, vol. 60, no. 1, pp. 1084-1087, 1999, ISSN: 1063-651X.
Abstract | BibTeX | Tags: | Links:
@article{sbs99,
title = {Structure of supercooled and glassy water under pressure},
author = {Starr, Francis W. and Bellissent-Funel, Mairie Claire and Stanley, H. Eugene},
url = {http://fstarr.web.wesleyan.edu/publications/sbs.pdf},
doi = {10.1103/PhysRevE.60.1084},
issn = {1063-651X},
year = {1999},
date = {1999-07-01},
journal = {PHYSICAL REVIEW E},
volume = {60},
number = {1},
pages = {1084-1087},
abstract = {We use molecular-dynamics simulations to study the effect of temperature and pressure on the local structure of liquid water in parallel with neutron-scattering experiments. We find, in agreement with experimental results, that the simulated liquid structure at high pressure is nearly independent of temperature, and remarkably similar to the known structure of the high-density amorphous ice. Further, at low pressure, the liquid structure appears to approach the experimentally measured structure of low-density amorphous ice as temperature decreases. These results are consistent with the postulated continuity between the liquid and glassy phases of H2O. [S1063-651X(99)10007-2].},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We use molecular-dynamics simulations to study the effect of temperature and pressure on the local structure of liquid water in parallel with neutron-scattering experiments. We find, in agreement with experimental results, that the simulated liquid structure at high pressure is nearly independent of temperature, and remarkably similar to the known structure of the high-density amorphous ice. Further, at low pressure, the liquid structure appears to approach the experimentally measured structure of low-density amorphous ice as temperature decreases. These results are consistent with the postulated continuity between the liquid and glassy phases of H2O. [S1063-651X(99)10007-2].
Starr, Francis W; Harrington, S; Sciortino, Francesco; Stanley, Eugene H
Slow dynamics of water under pressure Journal Article
In: PHYSICAL REVIEW LETTERS, vol. 82, no. 18, pp. 3629-3632, 1999, ISSN: 0031-9007.
Abstract | BibTeX | Tags: | Links:
@article{shss99b,
title = {Slow dynamics of water under pressure},
author = {Francis W Starr and S Harrington and Francesco Sciortino and Eugene H Stanley},
url = {http://fstarr.web.wesleyan.edu/publications/shss.pdf},
doi = {10.1103/PhysRevLett.82.3629},
issn = {0031-9007},
year = {1999},
date = {1999-05-01},
journal = {PHYSICAL REVIEW LETTERS},
volume = {82},
number = {18},
pages = {3629-3632},
abstract = {We perform lengthy molecular dynamics simulations to investigate the
dynamics of water under pressure at many temperatures and compare with
experimental measurements. We calculate the isochrones of the diffusion
constant D and find, as observed experimentally, power-law behavior of D
as temperature approaches T-c(P). We find that the dynamics are
consistent with slowing down due to the transient caging of molecules,
as described by the mode-coupling theory (MCT). This supports the
hypothesis that the apparent divergences of dynamic quantities along the
line T-c(P) in water may be associated with ``slowing down'' as
predicted by MCT. [S0031-9007(99)09047-X].},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We perform lengthy molecular dynamics simulations to investigate the
dynamics of water under pressure at many temperatures and compare with
experimental measurements. We calculate the isochrones of the diffusion
constant D and find, as observed experimentally, power-law behavior of D
as temperature approaches T-c(P). We find that the dynamics are
consistent with slowing down due to the transient caging of molecules,
as described by the mode-coupling theory (MCT). This supports the
hypothesis that the apparent divergences of dynamic quantities along the
line T-c(P) in water may be associated with ``slowing down'' as
predicted by MCT. [S0031-9007(99)09047-X].
dynamics of water under pressure at many temperatures and compare with
experimental measurements. We calculate the isochrones of the diffusion
constant D and find, as observed experimentally, power-law behavior of D
as temperature approaches T-c(P). We find that the dynamics are
consistent with slowing down due to the transient caging of molecules,
as described by the mode-coupling theory (MCT). This supports the
hypothesis that the apparent divergences of dynamic quantities along the
line T-c(P) in water may be associated with ``slowing down'' as
predicted by MCT. [S0031-9007(99)09047-X].
Starr, Francis W.; Harrington, S; Sciortino, Francesco; Stanley, H. Eugene
Slow dynamics of water under pressure Journal Article
In: PHYSICAL REVIEW LETTERS, vol. 82, no. 18, pp. 3629-3632, 1999, ISSN: 0031-9007.
Abstract | BibTeX | Tags: | Links:
@article{shss99,
title = {Slow dynamics of water under pressure},
author = {Starr, Francis W. and Harrington, S and Sciortino, Francesco and Stanley, H. Eugene},
url = {http://fstarr.web.wesleyan.edu/publications/shss.pdf},
doi = {10.1103/PhysRevLett.82.3629},
issn = {0031-9007},
year = {1999},
date = {1999-05-01},
journal = {PHYSICAL REVIEW LETTERS},
volume = {82},
number = {18},
pages = {3629-3632},
abstract = {We perform lengthy molecular dynamics simulations to investigate the dynamics of water under pressure at many temperatures and compare with experimental measurements. We calculate the isochrones of the diffusion constant D and find, as observed experimentally, power-law behavior of D as temperature approaches T-c(P). We find that the dynamics are consistent with slowing down due to the transient caging of molecules, as described by the mode-coupling theory (MCT). This supports the hypothesis that the apparent divergences of dynamic quantities along the line T-c(P) in water may be associated with ``slowing down'' as predicted by MCT. [S0031-9007(99)09047-X].},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We perform lengthy molecular dynamics simulations to investigate the dynamics of water under pressure at many temperatures and compare with experimental measurements. We calculate the isochrones of the diffusion constant D and find, as observed experimentally, power-law behavior of D as temperature approaches T-c(P). We find that the dynamics are consistent with slowing down due to the transient caging of molecules, as described by the mode-coupling theory (MCT). This supports the hypothesis that the apparent divergences of dynamic quantities along the line T-c(P) in water may be associated with ``slowing down'' as predicted by MCT. [S0031-9007(99)09047-X].
Starr, Francis W; Nielsen, Johannes K; Stanley, Eugene H
Fast and slow dynamics of hydrogen bonds in liquid water Journal Article
In: PHYSICAL REVIEW LETTERS, vol. 82, no. 11, pp. 2294-2297, 1999, ISSN: 0031-9007.
Abstract | BibTeX | Tags: | Links:
@article{sns-prlb,
title = {Fast and slow dynamics of hydrogen bonds in liquid water},
author = {Francis W Starr and Johannes K Nielsen and Eugene H Stanley},
url = {http://fstarr.web.wesleyan.edu/publications/sns-prl.pdf},
doi = {10.1103/PhysRevLett.82.2294},
issn = {0031-9007},
year = {1999},
date = {1999-03-01},
journal = {PHYSICAL REVIEW LETTERS},
volume = {82},
number = {11},
pages = {2294-2297},
abstract = {We study hydrogen-bond dynamics in liquid water at low temperatures
using molecular dynamics simulations, and find results supporting the
hypothesized continuity of dynamic functions between the liquid and
glassy states of water. We find that average bond lifetime (similar to 1
ps) has Arrhenius temperature dependence. We also calculate the bond
correlation function decay time (similar to 1 ns) and find power-law
behavior consistent with the predictions of the mode-coupling theory,
suggesting that the slow dynamics of hydrogen bonds can be explained in
the same framework as standard transport quantities.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We study hydrogen-bond dynamics in liquid water at low temperatures
using molecular dynamics simulations, and find results supporting the
hypothesized continuity of dynamic functions between the liquid and
glassy states of water. We find that average bond lifetime (similar to 1
ps) has Arrhenius temperature dependence. We also calculate the bond
correlation function decay time (similar to 1 ns) and find power-law
behavior consistent with the predictions of the mode-coupling theory,
suggesting that the slow dynamics of hydrogen bonds can be explained in
the same framework as standard transport quantities.
using molecular dynamics simulations, and find results supporting the
hypothesized continuity of dynamic functions between the liquid and
glassy states of water. We find that average bond lifetime (similar to 1
ps) has Arrhenius temperature dependence. We also calculate the bond
correlation function decay time (similar to 1 ns) and find power-law
behavior consistent with the predictions of the mode-coupling theory,
suggesting that the slow dynamics of hydrogen bonds can be explained in
the same framework as standard transport quantities.
Starr, Francis W.; Nielsen, Johannes K.; Stanley, H. Eugene
Fast and slow dynamics of hydrogen bonds in liquid water Journal Article
In: PHYSICAL REVIEW LETTERS, vol. 82, no. 11, pp. 2294-2297, 1999, ISSN: 0031-9007.
Abstract | BibTeX | Tags: | Links:
@article{sns-prl,
title = {Fast and slow dynamics of hydrogen bonds in liquid water},
author = {Starr, Francis W. and Nielsen, Johannes K. and Stanley, H. Eugene},
url = {http://fstarr.web.wesleyan.edu/publications/sns-prl.pdf},
doi = {10.1103/PhysRevLett.82.2294},
issn = {0031-9007},
year = {1999},
date = {1999-03-01},
journal = {PHYSICAL REVIEW LETTERS},
volume = {82},
number = {11},
pages = {2294-2297},
abstract = {We study hydrogen-bond dynamics in liquid water at low temperatures using molecular dynamics simulations, and find results supporting the hypothesized continuity of dynamic functions between the liquid and glassy states of water. We find that average bond lifetime (similar to 1 ps) has Arrhenius temperature dependence. We also calculate the bond correlation function decay time (similar to 1 ns) and find power-law behavior consistent with the predictions of the mode-coupling theory, suggesting that the slow dynamics of hydrogen bonds can be explained in the same framework as standard transport quantities.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We study hydrogen-bond dynamics in liquid water at low temperatures using molecular dynamics simulations, and find results supporting the hypothesized continuity of dynamic functions between the liquid and glassy states of water. We find that average bond lifetime (similar to 1 ps) has Arrhenius temperature dependence. We also calculate the bond correlation function decay time (similar to 1 ns) and find power-law behavior consistent with the predictions of the mode-coupling theory, suggesting that the slow dynamics of hydrogen bonds can be explained in the same framework as standard transport quantities.
1998
Canpolat, Murat; Starr, Francis W; Scala, Antonio; Sadr-Lahijany, MR; Mishima, Osamu; Havlin, Shlomo; Stanley, Eugene H
Local structural heterogeneities in liquid water under pressure Journal Article
In: CHEMICAL PHYSICS LETTERS, vol. 294, no. 1-3, pp. 9-12, 1998, ISSN: 0009-2614.
Abstract | BibTeX | Tags: | Links:
@article{csssmhsb,
title = {Local structural heterogeneities in liquid water under pressure},
author = {Murat Canpolat and Francis W Starr and Antonio Scala and MR Sadr-Lahijany and Osamu Mishima and Shlomo Havlin and Eugene H Stanley},
url = {http://fstarr.web.wesleyan.edu/publications/csssmhs.pdf},
doi = {10.1016/S0009-2614(98)00828-8},
issn = {0009-2614},
year = {1998},
date = {1998-09-01},
journal = {CHEMICAL PHYSICS LETTERS},
volume = {294},
number = {1-3},
pages = {9-12},
abstract = {We investigate the local structural heterogeneities that may appear in
liquid water by studying a model of interacting water pentamers, We find
local energy minima which we identify with well-defined configurations,
and advance the hypothesis that one of these configurations may be
related to local ``high-density'' structural heterogeneities occurring
in liquid water when subjected to high pressure. Our results are
consistent with experimental data on the effect of high pressure on the
radial distribution function, and are further tested by molecular
dynamics simulations reported here. (C) 1998 Published by Elsevier
Science B,V. All rights reserved.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We investigate the local structural heterogeneities that may appear in
liquid water by studying a model of interacting water pentamers, We find
local energy minima which we identify with well-defined configurations,
and advance the hypothesis that one of these configurations may be
related to local ``high-density'' structural heterogeneities occurring
in liquid water when subjected to high pressure. Our results are
consistent with experimental data on the effect of high pressure on the
radial distribution function, and are further tested by molecular
dynamics simulations reported here. (C) 1998 Published by Elsevier
Science B,V. All rights reserved.
liquid water by studying a model of interacting water pentamers, We find
local energy minima which we identify with well-defined configurations,
and advance the hypothesis that one of these configurations may be
related to local ``high-density'' structural heterogeneities occurring
in liquid water when subjected to high pressure. Our results are
consistent with experimental data on the effect of high pressure on the
radial distribution function, and are further tested by molecular
dynamics simulations reported here. (C) 1998 Published by Elsevier
Science B,V. All rights reserved.
Canpolat, Murat; Starr, Francis W.; Scala, Antonio; Sadr-Lahijany, MR; Mishima, Osamu; Havlin, Shlomo; Stanley, H. Eugene
Local structural heterogeneities in liquid water under pressure Journal Article
In: CHEMICAL PHYSICS LETTERS, vol. 294, no. 1-3, pp. 9-12, 1998, ISSN: 0009-2614.
Abstract | BibTeX | Tags: | Links:
@article{csssmhs,
title = {Local structural heterogeneities in liquid water under pressure},
author = {Canpolat, Murat and Starr, Francis W. and Scala, Antonio and Sadr-Lahijany, MR and Mishima, Osamu and Havlin, Shlomo and Stanley, H. Eugene},
url = {http://fstarr.web.wesleyan.edu/publications/csssmhs.pdf},
doi = {10.1016/S0009-2614(98)00828-8},
issn = {0009-2614},
year = {1998},
date = {1998-09-01},
journal = {CHEMICAL PHYSICS LETTERS},
volume = {294},
number = {1-3},
pages = {9-12},
abstract = {We investigate the local structural heterogeneities that may appear in liquid water by studying a model of interacting water pentamers, We find local energy minima which we identify with well-defined configurations, and advance the hypothesis that one of these configurations may be related to local ``high-density'' structural heterogeneities occurring in liquid water when subjected to high pressure. Our results are consistent with experimental data on the effect of high pressure on the radial distribution function, and are further tested by molecular dynamics simulations reported here. (C) 1998 Published by Elsevier Science B,V. All rights reserved.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
We investigate the local structural heterogeneities that may appear in liquid water by studying a model of interacting water pentamers, We find local energy minima which we identify with well-defined configurations, and advance the hypothesis that one of these configurations may be related to local ``high-density'' structural heterogeneities occurring in liquid water when subjected to high pressure. Our results are consistent with experimental data on the effect of high pressure on the radial distribution function, and are further tested by molecular dynamics simulations reported here. (C) 1998 Published by Elsevier Science B,V. All rights reserved.
Stanley, Eugene H; Buldyrev, Sergey V; Canpolat, Murat; Meyer, Martin; Mishima, Osamu; Sadr-Lahijany, MR; Scala, Antonio; Starr, Francis W
The puzzling statistical physics of liquid water Journal Article
In: PHYSICA A-STATISTICAL MECHANICS AND ITS APPLICATIONS, vol. 257, no. 1-4, pp. 213-232, 1998, ISSN: 0378-4371, (Vth Latin American Workshop on Non-Linear Phenomena/11th MEDYFINOL Conference on Statistical Physics of Dynamic and Complex Systems, CANELA, BRAZIL, SEP 28-OCT 03, 1997).
Abstract | BibTeX | Tags: | Links:
@article{review98b,
title = {The puzzling statistical physics of liquid water},
author = {Eugene H Stanley and Sergey V Buldyrev and Murat Canpolat and Martin Meyer and Osamu Mishima and MR Sadr-Lahijany and Antonio Scala and Francis W Starr},
url = {http://fstarr.web.wesleyan.edu/publications/review98.pdf},
doi = {10.1016/S0378-4371(98)00264-7},
issn = {0378-4371},
year = {1998},
date = {1998-08-01},
journal = {PHYSICA A-STATISTICAL MECHANICS AND ITS APPLICATIONS},
volume = {257},
number = {1-4},
pages = {213-232},
abstract = {Although H(2)O has been the topic of considerable research since the
beginning of the century, the peculiar physical properties are still not
well understood. We discuss recent experiments and simulations relating
to the hypothesis that, in addition to the known critical point in
water, there exists a ``second'' critical point at low temperatures.
in particular, we discuss very recent measurements of the
compression-induced melting and decompression-induced melting lines of
high-pressure forms of ice. We show how knowledge of these lines enables
one to obtain an approximation for the Gibbs potential G(P, T) and the
equation of state V/(P, T) for water, both of which are consistent with
the possible continuity of liquid water and the amorphous forms of solid
water. We also comment on some of the evidence that is equally
consistent with other scenarios for the behavior of liquid water. (C)
1998 Elsevier Science B.V. All rights reserved.},
note = {Vth Latin American Workshop on Non-Linear Phenomena/11th MEDYFINOL
Conference on Statistical Physics of Dynamic and Complex Systems,
CANELA, BRAZIL, SEP 28-OCT 03, 1997},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Although H(2)O has been the topic of considerable research since the
beginning of the century, the peculiar physical properties are still not
well understood. We discuss recent experiments and simulations relating
to the hypothesis that, in addition to the known critical point in
water, there exists a ``second'' critical point at low temperatures.
in particular, we discuss very recent measurements of the
compression-induced melting and decompression-induced melting lines of
high-pressure forms of ice. We show how knowledge of these lines enables
one to obtain an approximation for the Gibbs potential G(P, T) and the
equation of state V/(P, T) for water, both of which are consistent with
the possible continuity of liquid water and the amorphous forms of solid
water. We also comment on some of the evidence that is equally
consistent with other scenarios for the behavior of liquid water. (C)
1998 Elsevier Science B.V. All rights reserved.
beginning of the century, the peculiar physical properties are still not
well understood. We discuss recent experiments and simulations relating
to the hypothesis that, in addition to the known critical point in
water, there exists a ``second'' critical point at low temperatures.
in particular, we discuss very recent measurements of the
compression-induced melting and decompression-induced melting lines of
high-pressure forms of ice. We show how knowledge of these lines enables
one to obtain an approximation for the Gibbs potential G(P, T) and the
equation of state V/(P, T) for water, both of which are consistent with
the possible continuity of liquid water and the amorphous forms of solid
water. We also comment on some of the evidence that is equally
consistent with other scenarios for the behavior of liquid water. (C)
1998 Elsevier Science B.V. All rights reserved.
Stanley, H. Eugene; Buldyrev, Sergey V.; Canpolat, Murat; Meyer, Martin; Mishima, Osamu; Sadr-Lahijany, MR; Scala, Antonio; Starr, Francis W.
The puzzling statistical physics of liquid water Journal Article
In: PHYSICA A-STATISTICAL MECHANICS AND ITS APPLICATIONS, vol. 257, no. 1-4, pp. 213-232, 1998, ISSN: 0378-4371, (Vth Latin American Workshop on Non-Linear Phenomena/11th MEDYFINOL Conference on Statistical Physics of Dynamic and Complex Systems, CANELA, BRAZIL, SEP 28-OCT 03, 1997).
Abstract | BibTeX | Tags: | Links:
@article{review98,
title = {The puzzling statistical physics of liquid water},
author = {Stanley, H. Eugene and Buldyrev, Sergey V. and Canpolat, Murat and Meyer, Martin and Mishima, Osamu and Sadr-Lahijany, MR and Scala, Antonio and Starr, Francis W.},
url = {http://fstarr.web.wesleyan.edu/publications/review98.pdf},
doi = {10.1016/S0378-4371(98)00264-7},
issn = {0378-4371},
year = {1998},
date = {1998-08-01},
journal = {PHYSICA A-STATISTICAL MECHANICS AND ITS APPLICATIONS},
volume = {257},
number = {1-4},
pages = {213-232},
abstract = {Although H(2)O has been the topic of considerable research since the beginning of the century, the peculiar physical properties are still not well understood. We discuss recent experiments and simulations relating to the hypothesis that, in addition to the known critical point in water, there exists a ``second'' critical point at low temperatures. in particular, we discuss very recent measurements of the compression-induced melting and decompression-induced melting lines of high-pressure forms of ice. We show how knowledge of these lines enables one to obtain an approximation for the Gibbs potential G(P, T) and the equation of state V/(P, T) for water, both of which are consistent with the possible continuity of liquid water and the amorphous forms of solid water. We also comment on some of the evidence that is equally consistent with other scenarios for the behavior of liquid water. (C) 1998 Elsevier Science B.V. All rights reserved.},
note = {Vth Latin American Workshop on Non-Linear Phenomena/11th MEDYFINOL Conference on Statistical Physics of Dynamic and Complex Systems, CANELA, BRAZIL, SEP 28-OCT 03, 1997},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Although H(2)O has been the topic of considerable research since the beginning of the century, the peculiar physical properties are still not well understood. We discuss recent experiments and simulations relating to the hypothesis that, in addition to the known critical point in water, there exists a ``second'' critical point at low temperatures. in particular, we discuss very recent measurements of the compression-induced melting and decompression-induced melting lines of high-pressure forms of ice. We show how knowledge of these lines enables one to obtain an approximation for the Gibbs potential G(P, T) and the equation of state V/(P, T) for water, both of which are consistent with the possible continuity of liquid water and the amorphous forms of solid water. We also comment on some of the evidence that is equally consistent with other scenarios for the behavior of liquid water. (C) 1998 Elsevier Science B.V. All rights reserved.
1996
Starr, Francis W; Harrington, Stephen T; Boghosian, Bruce M; Stanley, Eugene H
Interface roughening in a hydrodynamic lattice-gas model with surfactant Journal Article
In: PHYSICAL REVIEW LETTERS, vol. 77, no. 16, pp. 3363-3366, 1996, ISSN: 0031-9007.
Abstract | BibTeX | Tags: | Links:
@article{shbs96b,
title = {Interface roughening in a hydrodynamic lattice-gas model with surfactant},
author = {Francis W Starr and Stephen T Harrington and Bruce M Boghosian and Eugene H Stanley},
url = {http://fstarr.web.wesleyan.edu/publications/shbs.pdf},
doi = {10.1103/PhysRevLett.77.3363},
issn = {0031-9007},
year = {1996},
date = {1996-10-01},
journal = {PHYSICAL REVIEW LETTERS},
volume = {77},
number = {16},
pages = {3363-3366},
abstract = {Using a hydrodynamic lattice-gas model, we study interface growth in a
binary fluid with various concentrations of surfactant. We find that the
interface is smoothed by small concentrations of surfactant, while
microemulsion droplets form for large surfactant concentrations. To
assist in determining the stability limits of the interface, we
calculate the change in the roughness and growth exponents ct and beta
as a function of surfactant concentration along the interface.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Using a hydrodynamic lattice-gas model, we study interface growth in a
binary fluid with various concentrations of surfactant. We find that the
interface is smoothed by small concentrations of surfactant, while
microemulsion droplets form for large surfactant concentrations. To
assist in determining the stability limits of the interface, we
calculate the change in the roughness and growth exponents ct and beta
as a function of surfactant concentration along the interface.
binary fluid with various concentrations of surfactant. We find that the
interface is smoothed by small concentrations of surfactant, while
microemulsion droplets form for large surfactant concentrations. To
assist in determining the stability limits of the interface, we
calculate the change in the roughness and growth exponents ct and beta
as a function of surfactant concentration along the interface.
Starr, Francis W.; Harrington, Stephen T.; Boghosian, Bruce M.; Stanley, H. Eugene
Interface roughening in a hydrodynamic lattice-gas model with surfactant Journal Article
In: PHYSICAL REVIEW LETTERS, vol. 77, no. 16, pp. 3363-3366, 1996, ISSN: 0031-9007.
Abstract | BibTeX | Tags: | Links:
@article{shbs96,
title = {Interface roughening in a hydrodynamic lattice-gas model with surfactant},
author = {Starr, Francis W. and Harrington, Stephen T. and Boghosian, Bruce M. and Stanley, H. Eugene},
url = {http://fstarr.web.wesleyan.edu/publications/shbs.pdf},
doi = {10.1103/PhysRevLett.77.3363},
issn = {0031-9007},
year = {1996},
date = {1996-10-01},
journal = {PHYSICAL REVIEW LETTERS},
volume = {77},
number = {16},
pages = {3363-3366},
abstract = {Using a hydrodynamic lattice-gas model, we study interface growth in a binary fluid with various concentrations of surfactant. We find that the interface is smoothed by small concentrations of surfactant, while microemulsion droplets form for large surfactant concentrations. To assist in determining the stability limits of the interface, we calculate the change in the roughness and growth exponents ct and beta as a function of surfactant concentration along the interface.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Using a hydrodynamic lattice-gas model, we study interface growth in a binary fluid with various concentrations of surfactant. We find that the interface is smoothed by small concentrations of surfactant, while microemulsion droplets form for large surfactant concentrations. To assist in determining the stability limits of the interface, we calculate the change in the roughness and growth exponents ct and beta as a function of surfactant concentration along the interface.