Published September 17, 2024 | Version v1
Journal article

Irreversible Boltzmann samplers in dense liquids: Weak-coupling approximation and mode-coupling theory

  • 1. Laboratoire Matière et Systèmes Complexes (MSC), Université Paris Cité and CNRS (UMR 7057), 75013 Paris, France
  • 2. Laboratoire Charles Coulomb (L2C), Université de Montpellier and CNRS (UMR 5221), 34095 Montpellier, France
  • 3. Gulliver, UMR CNRS 7083, ESPCI Paris, PSL Research University, 75005 Paris, France
  • 4. Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, USA

Description

Exerting a nonequilibrium drive on an otherwise equilibrium Langevin process brings the dynamics out of equilibrium but can also speed up the approach to the Boltzmann steady state. Transverse forces are a minimal framework to achieve dynamical acceleration of the Boltzmann sampling. We consider a simple liquid in three space dimensions subjected to additional transverse pairwise forces, and quantify the extent to which transverse forces accelerate the dynamics. We first explore the dynamics of a tracer in a weak coupling regime describing high temperatures. The resulting acceleration is correlated with a monotonous increase of the magnitude of odd transport coefficients (mobility and diffusivity) with the amplitude of the transverse drive. We then develop a nonequilibrium version of the mode-coupling theory able to capture the effect of transverse forces, and more generally of forces created by additional degrees of freedom. Based on an analysis of transport coefficients, both odd and longitudinal, both for the collective modes and for a tracer particle, we find a systematic acceleration of the dynamics. Quantitatively, the gain, which is guaranteed throughout the ergodic phase, turns out to be a decreasing function of temperature beyond a temperature crossover, in particular as the glass transition is approached. Our theoretical results are in good agreement with available numerical results.

Additional details

Identifiers

DOI
10.1103/PhysRevE.110.034604;
arXiv
arXiv:2404.14863;
Crossref Funder ID
10.13039/501100001665; 10.13039/100000001;

Publishing Information

Journal Title
Physical Review E
Journal Volume
110
Journal Issue
3
Journal Page Range
28 pgs.
ISSN
1089-3787

Optional Information

Copyright
©2024 American Physical Society
Contract/Grant/Project number
THEMA AAPG2020; CHE 2154241
Notes
Record automatically processed
Funding organization
Agence Nationale de la Recherche; National Science Foundation