Length-scale dependence of Stokes-Einstein breakdown in active glass-forming liquids

The Stokes-Einstein (SE) relation, which relates diffusion constants with the viscosity of a liquid at high temperatures in equilibrium, is violated in the supercooled temperature regime. Whether this relation is obeyed in nonequilibrium active liquids is a question of significant current interest to the statistical physics community trying to develop the theoretical framework of nonequilibrium statistical mechanics. Via extensive computer simulations of model active glass-forming liquids in three dimensions, we show that SE is obeyed at a high temperature similar to the equilibrium behavior, and it gets violated in the supercooled temperature regimes. The degree of violation increases systematically with the increasing activity which quantifies the amount the system is driven out of equilibrium. First passage-time (FPT) distributions helped us to gain insights into this enhanced breakdown from the increased short-time peak, depicting hoppers. Subsequently, we study the wave vector dependence of SE relation and show that it gets restored at a wave vector that decreases with increasing activity, and the crossover wave vector is found to be proportional to the inverse of the dynamical heterogeneity length scale in the system. Our work showed how SE violation in active supercooled liquids could be rationalized using the growth of dynamic length scale, which is found to grow enormously with increasing activity in these systems.

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Publication Details

Journal
Physical review. E
Published
2025-03-18
DOI
https://doi.org/10.1103/physreve.111.035409
Citations
1
Primary Topic
Material Dynamics and Properties
Type
article
Field-Weighted Citation Impact
0.52

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article

Length-scale dependence of Stokes-Einstein breakdown in active glass-forming liquids

Smarajit Karmakar, Anoop Mutneja
1 citations
Physical review. E
Material Dynamics and Properties
0.52
article

Length-scale dependence of Stokes-Einstein breakdown in active glass-forming liquids

Smarajit Karmakar, Anoop Mutneja
article en
1 citations

Abstract

The Stokes-Einstein (SE) relation, which relates diffusion constants with the viscosity of a liquid at high temperatures in equilibrium, is violated in the supercooled temperature regime. Whether this relation is obeyed in nonequilibrium active liquids is a question of significant current interest to the statistical physics community trying to develop the theoretical framework of nonequilibrium statistical mechanics. Via extensive computer simulations of model active glass-forming liquids in three dimensions, we show that SE is obeyed at a high temperature similar to the equilibrium behavior, and it gets violated in the supercooled temperature regimes. The degree of violation increases systematically with the increasing activity which quantifies the amount the system is driven out of equilibrium. First passage-time (FPT) distributions helped us to gain insights into this enhanced breakdown from the increased short-time peak, depicting hoppers. Subsequently, we study the wave vector dependence of SE relation and show that it gets restored at a wave vector that decreases with increasing activity, and the crossover wave vector is found to be proportional to the inverse of the dynamical heterogeneity length scale in the system. Our work showed how SE violation in active supercooled liquids could be rationalized using the growth of dynamic length scale, which is found to grow enormously with increasing activity in these systems.

Physical review. EVol. 111(3)
Tata Institute of Fundamental Research (IN)
Department of Atomic Energy, Government of India, Science and Engineering Research Board
Openalex Percentile: Top 41%
Material Dynamics and Properties
0.52
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