Dissipative systems often exhibit novel and unexpected properties. This is, for instance, the case of simple liquids, which, when subjected to shear and after reaching a steady state, can exhibit a negative entropy production over finite length scales and timescales. This result, among others, is captured by nonequilibrium relations known as fluctuation theorems. Using nonequilibrium molecular dynamics simulations, we examine how, by fine-tuning the properties of the components of a complex fluid, we can steer the nonequilibrium response of the fluid. More specifically, we show how we control the nonequilibrium probability distribution for the shear stress and, in turn, how often states with a negative entropy production can occur. To achieve this, we start by characterizing how the size for the liquid matrix impacts the probability of observing negative entropy states, as well as the timescale over which these can be observed. We then measure how the addition of larger particles to this liquid matrix, i.e., simulating a model colloidal suspension, results in an increase in the occurrence of such states. This suggests how modifications in the composition of the mixture and in the properties of its components lead to an increase in the probability of observing states of negative entropy production and, thus, for the system to run in reverse.
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14 December 2020
Research Article|
December 09 2020
Entropy production in model colloidal suspensions under shear via the fluctuation theorem
Caroline Desgranges
;
Caroline Desgranges
Department of Chemistry, New York University
, New York, New York 10003, USA
and Department of Chemistry & Molecular Simulation of NonEquilibrium Processes (MSNEP), Suite 2300, Tech Accelerator, University of North Dakota
, Grand Forks, North Dakota 58202, USA
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Jerome Delhommelle
Jerome Delhommelle
a)
Department of Chemistry, New York University
, New York, New York 10003, USA
and Department of Chemistry & Molecular Simulation of NonEquilibrium Processes (MSNEP), Suite 2300, Tech Accelerator, University of North Dakota
, Grand Forks, North Dakota 58202, USA
a)Author to whom correspondence should be addressed: [email protected]
Search for other works by this author on:
a)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 153, 224113 (2020)
Article history
Received:
August 19 2020
Accepted:
November 23 2020
Citation
Caroline Desgranges, Jerome Delhommelle; Entropy production in model colloidal suspensions under shear via the fluctuation theorem. J. Chem. Phys. 14 December 2020; 153 (22): 224113. https://doi.org/10.1063/5.0025954
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