This paper studies size-polydisperse Lennard-Jones systems described by active Ornstein-Uhlenbeck... more This paper studies size-polydisperse Lennard-Jones systems described by active Ornstein-Uhlenbeck particle dynamics. The focus is on the existence of isomorphs (curves of invariant structure and dynamics) in the model's three-dimensional phase diagram. Isomorphs are traced out from a single steady-state configuration by means of the configurational-temperature method. Good invariance of the reduced-unit radial distribution function and the mean-square displacement as a function of time is demonstrated for three uniform-distribution polydispersities, 12%, 23%, and 29%. Comparing to active-matter isomorphs generated by the analytical direct-isomorph-check method, the latter give somewhat poorer invariance of the structure, but better invariance of the dynamics. We conclude that both methods can be used to quickly get an overview of the phase diagram of polydisperse AOUP models involving a potential-energy function obeying the hiddenscale-invariance property required for isomorph theory to apply.
Active-matter isomorphs in the size-polydisperse Ornstein–Uhlenbeck Lennard–Jones model
Journal of Physics: Condensed Matter
This paper studies size-polydisperse Lennard–Jones systems described by active Ornstein–Uhlenbeck... more This paper studies size-polydisperse Lennard–Jones systems described by active Ornstein–Uhlenbeck particle (AOUP) dynamics. The focus is on the existence of isomorphs (curves of invariant structure and dynamics) in the model’s three-dimensional phase diagram. Isomorphs are traced out from a single steady-state configuration by means of the configurational-temperature method. Good isomorph invariance of the reduced-unit radial distribution function and the mean-square displacement as a function of time is demonstrated for three uniform-distribution polydispersities, 12 % , 23%, and 29%. Comparing to active-matter isomorphs generated by the analytical direct-isomorph-check method, the latter have poorer invariance of the structure, but better invariance of the dynamics. We conclude that both methods can be used to quickly get an overview of the phase diagram of polydisperse AOUP models involving a potential-energy function obeying the hidden-scale-invariance property required for isom...
We show that the liquid-state-theory configurational temperature T conf defines an energy scale, ... more We show that the liquid-state-theory configurational temperature T conf defines an energy scale, which for dry active-matter models can be used to determine how to adjust model parameters to achieve approximately invariant structure and dynamics when density is changed. The required parameter changes are calculated from the variation of a single configuration's T conf upon a uniform scaling of all coordinates. The formalism developed applies for models involving a potentialenergy function with hidden scale invariance. The procedure is illustrated by computer simulations of the Kob-Andersen binary Lennard-Jones model with active Ornstein-Uhlenbeck dynamics in three dimensions and the two-dimensional single-component Yukawa model with active Brownian particle dynamics. For the latter model we also show how T conf may be applied for estimating the MIPS phase boundary, in effect reducing by one the dimension of the parameter space. We finally propose that the ratio between the equilibrium-system temperature corresponding to actual potential energy and T conf provides a useful measure of how far an active-matter system is from thermal equilibrium.
We analyse the flow curves of a two-dimensional assembly of granular particles which are interact... more We analyse the flow curves of a two-dimensional assembly of granular particles which are interacting via frictional contact forces. For packing fractions slightly below jamming, the fluid undergoes a large scale instability, implying a range of stress and strainrates where no stationary flow can exist. Whereas small systems were shown previously to exhibit hysteretic jumps between the low and high stress branches, large systems exhibit continuous shear thickening arising from averaging unsteady, spatially heterogeneous flows. The observed large scale patterns as well as their dynamics are found to depend on strainrate: At the lower end of the unstable region, force chains merge to form giant bands that span the system in compressional direction and propagate in dilational direction. At the upper end, we observe large scale clusters which extend along the dilational direction and propagate along the compressional direction. Both patterns, bands and clusters, come in with infinite cor...
When a binary liquid is confined by a strongly repulsive wall, the local density is depleted near... more When a binary liquid is confined by a strongly repulsive wall, the local density is depleted near the wall and an interface similar to that between the liquid and its vapor is formed. This analogy suggests that the composition of the binary liquid near this interface should exhibit spatial modulation similar to that near a liquid-vapor interface even if the interactions of the wall with the two components of the liquid are the same. The Guggenheim adsorption relation quantifies the concentrations of two components of a binary mixture near a liquid-vapor interface and qualitatively states that the majority (minority) component enriches the interface for negative (positive) mixing energy if the surface tensions of the two components are not very different. From molecular dynamics simulations of binary mixtures with different compositions and interactions, we find that the Guggenheim relation is qualitatively satisfied at wall-induced interfaces for systems with negative mixing energy ...
Motivated by the formal argument that a non-zero shear modulus is the result of averaging over a ... more Motivated by the formal argument that a non-zero shear modulus is the result of averaging over a constrained configurations space, we demonstrate that the shear modulus calculated over a range of temperatures and averaging times can be expressed (relative to its infinite frequency value) as a single function of the mean squared displacement. This result is shown to hold for both a glass-liquid and a crystal-liquid system.
We demonstrate that irreversible structural reorganization is not necessary for the observation o... more We demonstrate that irreversible structural reorganization is not necessary for the observation of yield behaviour in an amorphous solid. While the majority of solids strained to their yield point do indeed undergo an irreversible reorganization, we find a significant fraction of solids exhibit yield via a reversible strain. We also demonstrate that large instantaneous strains in excess of the yield stress can result in complete stress relaxation, a result of the large non-affine motions driven by the applied strain. The empirical similarity of the dependence of the ratio of stress over strain on the non-affine mean squared displacement with that for the shear modulus obtained from quiescent liquid at non-zero temperature supports the proposition that rigidity depends on the size of the sampled configurational space only, and is insensitive as to how this space is sampled.
It is proposed that the rate of relaxation in a liquid is better described by the geometric mean ... more It is proposed that the rate of relaxation in a liquid is better described by the geometric mean of the van Hove distribution function, rather than the standard arithmetic mean used to obtain the mean squared displacement. The difference between the two means is shown to increase significantly with an increase in the non-Gaussian character of the displacement distribution. Preliminary results indicate that the geometric diffusion constant results in a substantial reduction of the deviation from Stokes-Einstein scaling.
Physical review. E, Statistical, nonlinear, and soft matter physics, 2015
When a binary liquid is confined by a strongly repulsive wall, the local density is depleted near... more When a binary liquid is confined by a strongly repulsive wall, the local density is depleted near the wall and an interface similar to that between the liquid and its vapor is formed. This analogy suggests that the composition of the binary liquid near this interface should exhibit spatial modulation similar to that near a liquid-vapor interface even if the interactions of the wall with the two components of the liquid are the same. The Guggenheim adsorption relation quantifies the concentrations of two components of a binary mixture near a liquid-vapor interface and qualitatively states that the majority (minority) component enriches the interface for negative (positive) mixing energy if the surface tensions of the two components are not very different. From molecular dynamics simulations of binary mixtures with different compositions and interactions we find that the Guggenheim relation is qualitatively satisfied at wall-induced interfaces for systems with negative mixing energy a...
Motivated by the formal argument that a non-zero shear modulus is the result of averaging over a ... more Motivated by the formal argument that a non-zero shear modulus is the result of averaging over a constrained configurations space, we demonstrate that the shear modulus calculated over a range of temperatures and averaging times can be expressed (relative to its infinite frequency value) as a single function of the mean squared displacement. This result is shown to hold for both a glass-liquid and a crystal-liquid system.
In the condensed liquid phase, both single- and multicomponent Lennard–Jones (LJ) systems obey th... more In the condensed liquid phase, both single- and multicomponent Lennard–Jones (LJ) systems obey the “hidden-scale-invariance” symmetry to a good approximation. Defining an isomorph as a line of constant excess entropy in the thermodynamic phase diagram, the consequent approximate isomorph invariance of structure and dynamics in appropriate units is well documented. However, although all measures of the structure are predicted to be isomorph invariant, with few exceptions only the radial distribution function (RDF) has been investigated. This paper studies the variation along isomorphs of the nearest-neighbor geometry quantified by the occurrence of Voronoi structures, Frank–Kasper bonds, icosahedral local order, and bond-orientational order. Data are presented for the standard LJ system and for three binary LJ mixtures (Kob–Andersen, Wahnström, NiY2). We find that, while the nearest-neighbor geometry generally varies significantly throughout the phase diagram, good invariance is obse...
Combining the recent Piskulich-Thompson approach [Z. A. Piskulich and W. H. Thompson, J. Chem. Ph... more Combining the recent Piskulich-Thompson approach [Z. A. Piskulich and W. H. Thompson, J. Chem. Phys. 152, 011102 (2020)] with isomorph theory, from a single simulation the structure of a single-component Lennard-Jones (LJ) system is obtained at an arbitrary state point in almost the whole liquid region of the temperature-density phase diagram. The LJ system exhibits two temperature ranges where the van't Hoff assumption that energetic and entropic forces are temperature independent is valid to a good approximation. A method to evaluate the structure at an arbitrary state point along an isochore from the knowledge of structures at two temperatures on the isochore is also discussed. We argue that, in general, the structure of any hidden scale-invariant system obeying the van't Hoff assumption in the whole range of temperatures can be determined in the whole liquid region of the phase diagram from a single simulation.
We analyse the flow curves of a two-dimensional assembly of granular particles which are interact... more We analyse the flow curves of a two-dimensional assembly of granular particles which are interacting via frictional contact forces. For packing fractions slightly below jamming, the fluid undergoes a large scale instability, implying a range of stress and strainrates where no stationary flow can exist. Whereas small systems were shown previously to exhibit hysteretic jumps between the low and high stress branches, large systems exhibit continuous shear thickening arising from averaging unsteady, spatially heterogeneous flows. The observed large scale patterns as well as their dynamics are found to depend on strainrate: At the lower end of the unstable region, force chains merge to form giant bands that span the system in compressional direction and propagate in dilational direction. At the upper end, we observe large scale clusters which extend along the dilational direction and propagate along the compressional direction. Both patterns, bands and clusters, come in with infinite correlation length similar to the sudden onset of system-spanning plugs in impact experiments.
The enhancement of mobility at the surface of an amorphous alloy is studied using a combination o... more The enhancement of mobility at the surface of an amorphous alloy is studied using a combination of molecular dynamic simulations and normal mode analysis of the nonuniform distribution of Debye-Waller factors. The increased mobility at the surface is found to be associated with the appearance of Arrhenius temperature dependence. We show that the transverse Debye-Waller factor exhibits a peak at the surface. Over the accessible temperature range, we find that the bulk and surface diffusion coefficients obey the same empirical relationship with the respective Debye-Waller factors. Extrapolating this relationship to lower T, we argue that the observed decrease in the constraint at the surface is sufficient to account for the experimentally observed surface enhancement of mobility.
We demonstrate that irreversible structural reorganization is not necessary for the observation o... more We demonstrate that irreversible structural reorganization is not necessary for the observation of yield behaviour in an amorphous solid. While the majority of solids strained to their yield point do indeed undergo an irreversible reorganization, we find a significant fraction of solids exhibit yield via a reversible strain. We also demonstrate that large instantaneous strains in excess of the yield stress can result in complete stress relaxation, a result of the large nonaffine motions driven by the applied strain. The empirical similarity of the dependence of the ratio of stress over strain on the non-affine mean squared displacement with that for the shear modulus obtained from quiescent liquid at non-zero temperature supports the proposition that rigidity depends on the size of the sampled configurational space only, and is insensitive as to how this space is sampled.
This paper studies size-polydisperse Lennard-Jones systems described by active Ornstein-Uhlenbeck... more This paper studies size-polydisperse Lennard-Jones systems described by active Ornstein-Uhlenbeck particle dynamics. The focus is on the existence of isomorphs (curves of invariant structure and dynamics) in the model's three-dimensional phase diagram. Isomorphs are traced out from a single steady-state configuration by means of the configurational-temperature method. Good invariance of the reduced-unit radial distribution function and the mean-square displacement as a function of time is demonstrated for three uniform-distribution polydispersities, 12%, 23%, and 29%. Comparing to active-matter isomorphs generated by the analytical direct-isomorph-check method, the latter give somewhat poorer invariance of the structure, but better invariance of the dynamics. We conclude that both methods can be used to quickly get an overview of the phase diagram of polydisperse AOUP models involving a potential-energy function obeying the hiddenscale-invariance property required for isomorph theory to apply.
Active-matter isomorphs in the size-polydisperse Ornstein–Uhlenbeck Lennard–Jones model
Journal of Physics: Condensed Matter
This paper studies size-polydisperse Lennard–Jones systems described by active Ornstein–Uhlenbeck... more This paper studies size-polydisperse Lennard–Jones systems described by active Ornstein–Uhlenbeck particle (AOUP) dynamics. The focus is on the existence of isomorphs (curves of invariant structure and dynamics) in the model’s three-dimensional phase diagram. Isomorphs are traced out from a single steady-state configuration by means of the configurational-temperature method. Good isomorph invariance of the reduced-unit radial distribution function and the mean-square displacement as a function of time is demonstrated for three uniform-distribution polydispersities, 12 % , 23%, and 29%. Comparing to active-matter isomorphs generated by the analytical direct-isomorph-check method, the latter have poorer invariance of the structure, but better invariance of the dynamics. We conclude that both methods can be used to quickly get an overview of the phase diagram of polydisperse AOUP models involving a potential-energy function obeying the hidden-scale-invariance property required for isom...
We show that the liquid-state-theory configurational temperature T conf defines an energy scale, ... more We show that the liquid-state-theory configurational temperature T conf defines an energy scale, which for dry active-matter models can be used to determine how to adjust model parameters to achieve approximately invariant structure and dynamics when density is changed. The required parameter changes are calculated from the variation of a single configuration's T conf upon a uniform scaling of all coordinates. The formalism developed applies for models involving a potentialenergy function with hidden scale invariance. The procedure is illustrated by computer simulations of the Kob-Andersen binary Lennard-Jones model with active Ornstein-Uhlenbeck dynamics in three dimensions and the two-dimensional single-component Yukawa model with active Brownian particle dynamics. For the latter model we also show how T conf may be applied for estimating the MIPS phase boundary, in effect reducing by one the dimension of the parameter space. We finally propose that the ratio between the equilibrium-system temperature corresponding to actual potential energy and T conf provides a useful measure of how far an active-matter system is from thermal equilibrium.
We analyse the flow curves of a two-dimensional assembly of granular particles which are interact... more We analyse the flow curves of a two-dimensional assembly of granular particles which are interacting via frictional contact forces. For packing fractions slightly below jamming, the fluid undergoes a large scale instability, implying a range of stress and strainrates where no stationary flow can exist. Whereas small systems were shown previously to exhibit hysteretic jumps between the low and high stress branches, large systems exhibit continuous shear thickening arising from averaging unsteady, spatially heterogeneous flows. The observed large scale patterns as well as their dynamics are found to depend on strainrate: At the lower end of the unstable region, force chains merge to form giant bands that span the system in compressional direction and propagate in dilational direction. At the upper end, we observe large scale clusters which extend along the dilational direction and propagate along the compressional direction. Both patterns, bands and clusters, come in with infinite cor...
When a binary liquid is confined by a strongly repulsive wall, the local density is depleted near... more When a binary liquid is confined by a strongly repulsive wall, the local density is depleted near the wall and an interface similar to that between the liquid and its vapor is formed. This analogy suggests that the composition of the binary liquid near this interface should exhibit spatial modulation similar to that near a liquid-vapor interface even if the interactions of the wall with the two components of the liquid are the same. The Guggenheim adsorption relation quantifies the concentrations of two components of a binary mixture near a liquid-vapor interface and qualitatively states that the majority (minority) component enriches the interface for negative (positive) mixing energy if the surface tensions of the two components are not very different. From molecular dynamics simulations of binary mixtures with different compositions and interactions, we find that the Guggenheim relation is qualitatively satisfied at wall-induced interfaces for systems with negative mixing energy ...
Motivated by the formal argument that a non-zero shear modulus is the result of averaging over a ... more Motivated by the formal argument that a non-zero shear modulus is the result of averaging over a constrained configurations space, we demonstrate that the shear modulus calculated over a range of temperatures and averaging times can be expressed (relative to its infinite frequency value) as a single function of the mean squared displacement. This result is shown to hold for both a glass-liquid and a crystal-liquid system.
We demonstrate that irreversible structural reorganization is not necessary for the observation o... more We demonstrate that irreversible structural reorganization is not necessary for the observation of yield behaviour in an amorphous solid. While the majority of solids strained to their yield point do indeed undergo an irreversible reorganization, we find a significant fraction of solids exhibit yield via a reversible strain. We also demonstrate that large instantaneous strains in excess of the yield stress can result in complete stress relaxation, a result of the large non-affine motions driven by the applied strain. The empirical similarity of the dependence of the ratio of stress over strain on the non-affine mean squared displacement with that for the shear modulus obtained from quiescent liquid at non-zero temperature supports the proposition that rigidity depends on the size of the sampled configurational space only, and is insensitive as to how this space is sampled.
It is proposed that the rate of relaxation in a liquid is better described by the geometric mean ... more It is proposed that the rate of relaxation in a liquid is better described by the geometric mean of the van Hove distribution function, rather than the standard arithmetic mean used to obtain the mean squared displacement. The difference between the two means is shown to increase significantly with an increase in the non-Gaussian character of the displacement distribution. Preliminary results indicate that the geometric diffusion constant results in a substantial reduction of the deviation from Stokes-Einstein scaling.
Physical review. E, Statistical, nonlinear, and soft matter physics, 2015
When a binary liquid is confined by a strongly repulsive wall, the local density is depleted near... more When a binary liquid is confined by a strongly repulsive wall, the local density is depleted near the wall and an interface similar to that between the liquid and its vapor is formed. This analogy suggests that the composition of the binary liquid near this interface should exhibit spatial modulation similar to that near a liquid-vapor interface even if the interactions of the wall with the two components of the liquid are the same. The Guggenheim adsorption relation quantifies the concentrations of two components of a binary mixture near a liquid-vapor interface and qualitatively states that the majority (minority) component enriches the interface for negative (positive) mixing energy if the surface tensions of the two components are not very different. From molecular dynamics simulations of binary mixtures with different compositions and interactions we find that the Guggenheim relation is qualitatively satisfied at wall-induced interfaces for systems with negative mixing energy a...
Motivated by the formal argument that a non-zero shear modulus is the result of averaging over a ... more Motivated by the formal argument that a non-zero shear modulus is the result of averaging over a constrained configurations space, we demonstrate that the shear modulus calculated over a range of temperatures and averaging times can be expressed (relative to its infinite frequency value) as a single function of the mean squared displacement. This result is shown to hold for both a glass-liquid and a crystal-liquid system.
In the condensed liquid phase, both single- and multicomponent Lennard–Jones (LJ) systems obey th... more In the condensed liquid phase, both single- and multicomponent Lennard–Jones (LJ) systems obey the “hidden-scale-invariance” symmetry to a good approximation. Defining an isomorph as a line of constant excess entropy in the thermodynamic phase diagram, the consequent approximate isomorph invariance of structure and dynamics in appropriate units is well documented. However, although all measures of the structure are predicted to be isomorph invariant, with few exceptions only the radial distribution function (RDF) has been investigated. This paper studies the variation along isomorphs of the nearest-neighbor geometry quantified by the occurrence of Voronoi structures, Frank–Kasper bonds, icosahedral local order, and bond-orientational order. Data are presented for the standard LJ system and for three binary LJ mixtures (Kob–Andersen, Wahnström, NiY2). We find that, while the nearest-neighbor geometry generally varies significantly throughout the phase diagram, good invariance is obse...
Combining the recent Piskulich-Thompson approach [Z. A. Piskulich and W. H. Thompson, J. Chem. Ph... more Combining the recent Piskulich-Thompson approach [Z. A. Piskulich and W. H. Thompson, J. Chem. Phys. 152, 011102 (2020)] with isomorph theory, from a single simulation the structure of a single-component Lennard-Jones (LJ) system is obtained at an arbitrary state point in almost the whole liquid region of the temperature-density phase diagram. The LJ system exhibits two temperature ranges where the van't Hoff assumption that energetic and entropic forces are temperature independent is valid to a good approximation. A method to evaluate the structure at an arbitrary state point along an isochore from the knowledge of structures at two temperatures on the isochore is also discussed. We argue that, in general, the structure of any hidden scale-invariant system obeying the van't Hoff assumption in the whole range of temperatures can be determined in the whole liquid region of the phase diagram from a single simulation.
We analyse the flow curves of a two-dimensional assembly of granular particles which are interact... more We analyse the flow curves of a two-dimensional assembly of granular particles which are interacting via frictional contact forces. For packing fractions slightly below jamming, the fluid undergoes a large scale instability, implying a range of stress and strainrates where no stationary flow can exist. Whereas small systems were shown previously to exhibit hysteretic jumps between the low and high stress branches, large systems exhibit continuous shear thickening arising from averaging unsteady, spatially heterogeneous flows. The observed large scale patterns as well as their dynamics are found to depend on strainrate: At the lower end of the unstable region, force chains merge to form giant bands that span the system in compressional direction and propagate in dilational direction. At the upper end, we observe large scale clusters which extend along the dilational direction and propagate along the compressional direction. Both patterns, bands and clusters, come in with infinite correlation length similar to the sudden onset of system-spanning plugs in impact experiments.
The enhancement of mobility at the surface of an amorphous alloy is studied using a combination o... more The enhancement of mobility at the surface of an amorphous alloy is studied using a combination of molecular dynamic simulations and normal mode analysis of the nonuniform distribution of Debye-Waller factors. The increased mobility at the surface is found to be associated with the appearance of Arrhenius temperature dependence. We show that the transverse Debye-Waller factor exhibits a peak at the surface. Over the accessible temperature range, we find that the bulk and surface diffusion coefficients obey the same empirical relationship with the respective Debye-Waller factors. Extrapolating this relationship to lower T, we argue that the observed decrease in the constraint at the surface is sufficient to account for the experimentally observed surface enhancement of mobility.
We demonstrate that irreversible structural reorganization is not necessary for the observation o... more We demonstrate that irreversible structural reorganization is not necessary for the observation of yield behaviour in an amorphous solid. While the majority of solids strained to their yield point do indeed undergo an irreversible reorganization, we find a significant fraction of solids exhibit yield via a reversible strain. We also demonstrate that large instantaneous strains in excess of the yield stress can result in complete stress relaxation, a result of the large nonaffine motions driven by the applied strain. The empirical similarity of the dependence of the ratio of stress over strain on the non-affine mean squared displacement with that for the shear modulus obtained from quiescent liquid at non-zero temperature supports the proposition that rigidity depends on the size of the sampled configurational space only, and is insensitive as to how this space is sampled.
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