Related Experiment Video
Updated: Jun 10, 2025

Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics
Published on: April 12, 2019
Irreversible Boltzmann samplers in dense liquids: Weak-coupling approximation and mode-coupling theory
Federico Ghimenti1, Ludovic Berthier2,3, Grzegorz Szamel4
1<a href="https://ror.org/032w6q449">Laboratoire Matière et Systèmes Complexes (MSC)</a>, <a href="https://ror.org/05f82e368">Université Paris Cité</a> and CNRS (UMR 7057), 75013 Paris, France.
Abstract:
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.
Related Concept Videos
Distribution of Molecular Speeds
Real Gases: Effects of Intermolecular Forces and Molecular Volume Deriving Van der Waals Equation
IR Spectroscopy: Hooke's Law Approximation of Molecular Vibration
According to Hooke's law, the vibrational frequency is directly proportional to...
Spin–Spin Coupling Constant: Overview
Qualitatively, any spin plus-half nucleus polarizes the spins of its electrons to the minus-half state. Consequently, the paired electron in the hydrogen–carbon bond must...
Phase Transitions: Vaporization and Condensation
Molecular Comparison of Gases, Liquids, and Solids

