arXiv subjects

Jeetain Mittal

Publications and source records attributed to Jeetain Mittal.

22 records · Page 2Linked to original sources

arXiv2007

How short-range attractions impact the structural order, self-diffusivity, and viscosity of a fluid

We present molecular simulation data for viscosity, self-diffusivity, and the local structural ordering of (i) a hard-sphere fluid and (ii) a square-well fluid with short-range attractions. The latter fluid exhibits a region of dynamic anomalies in its phase diagram, where its mobility increases upon isochoric cooling, which is found to be a subset of a larger region of structural anomalies, in which its pair correlations strengthen upon isochoric heating. This "cascade of anomalies" qualitatively resembles that found in recent simulations of liquid water. The results for the hard-sphere and square-well systems also show that the breakdown of the Stokes-Einstein relation upon supercooling occurs for conditions where viscosity and self-diffusivity develop different couplings to the degree of pairwise structural ordering of the liquid. We discuss how these couplings reflect dynamic heterogeneities. Finally, we note that the simulation data suggests how repulsive and attractive glasses may generally be characterized by two distinct levels of short-range structural order.

cond-mat.soft↗

arXiv2006

Using Available Volume to Predict Fluid Diffusivity in Random Media

We propose a simple equation for predicting self-diffusivity of fluids embedded in random matrices of identical, but dynamically frozen, particles (i.e., quenched-annealed systems). The only nontrivial input is the volume available to mobile particles, which also can be predicted for two common matrix types that reflect equilibrium and non-equilibrium fluid structures. The proposed equation can account for the large differences in mobility exhibited by quenched-annealed systems with indistinguishable static pair correlations, illustrating the key role that available volume plays in transport.

cond-mat.stat-mech↗

arXiv2006

Relationship between thermodynamics and dynamics of supercooled liquids

Diffusivity, a measure for how rapidly a fluid self-mixes, shows an intimate, but seemingly fragmented, connection to thermodynamics. On one hand, the "configurational" contribution to entropy (related to the number of mechanically-stable configurations that fluid molecules can adopt) has long been considered key for predicting supercooled liquid dynamics near the glass transition. On the other hand, the excess entropy (relative to ideal gas) provides a robust scaling for the diffusivity of fluids above the freezing point. Here we provide, to our knowledge, the first evidence that excess entropy also captures how supercooling a fluid modifies its diffusivity, suggesting that dynamics, from ideal gas to glass, is related to a single, standard thermodynamic quantity.

cond-mat.stat-mech↗

arXiv2005

Thermodynamics predicts how confinement modifies hard-sphere dynamics

We study how confining the equilibrium hard-sphere fluid to restrictive one- and two-dimensional channels with smooth interacting walls modifies its structure, dynamics, and entropy using molecular dynamics and transition-matrix Monte Carlo simulations. Although confinement strongly affects local structuring, the relationships between self-diffusivity, excess entropy, and average fluid density are, to an excellent approximation, independent of channel width or particle-wall interactions. Thus, thermodynamics can be used to predict how confinement impacts dynamics.

cond-mat.stat-mech↗