1. Random force in molecular dynamics with electronic friction
- Author
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Dirk Schwarzer, Daniel J. Auerbach, Alec M. Wodtke, Raidel Martin-Barrios, Pascal Larrégaray, Alexander Kandratsenka, Oihana Galparsoro, Nils Hertl, Université de Bordeaux (UB), Institut des Sciences Moléculaires (ISM), and Université Montesquieu - Bordeaux 4-Université Sciences et Technologies - Bordeaux 1-École Nationale Supérieure de Chimie et de Physique de Bordeaux (ENSCPB)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)
- Subjects
Thermal fluctuations ,02 engineering and technology ,Thermal diffusivity ,01 natural sciences ,7. Clean energy ,Article ,Molecular dynamics ,0103 physical sciences ,Physical and Theoretical Chemistry ,010306 general physics ,Brownian motion ,ComputingMilieux_MISCELLANEOUS ,Physics ,business.industry ,Scattering ,021001 nanoscience & nanotechnology ,Surfaces, Coatings and Films ,Electronic, Optical and Magnetic Materials ,Langevin equation ,[CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry ,General Energy ,Classical mechanics ,Drag ,0210 nano-technology ,business ,Thermal energy - Abstract
Originally conceived to describe thermal diffusion, the Langevin equation includes both a frictional drag and a random force, the latter representing thermal fluctuations first seen as Brownian motion. The random force is crucial for the diffusion problem as it explains why friction does not simply bring the system to a standstill. When using the Langevin equation to describe ballistic motion, the importance of the random force is less obvious and it is often omitted, for example, in theoretical treatments of hot ions and atoms interacting with metals. Here, friction results from electronic nonadiabaticity (electronic friction), and the random force arises from thermal electron-hole pairs. We show the consequences of omitting the random force in the dynamics of H-atom scattering from metals. We compare molecular dynamics simulations based on the Langevin equation to experimentally derived energy loss distributions. Despite the fact that the incidence energy is much larger than the thermal energy and the scattering time is only about 25 fs, the energy loss distribution fails to reproduce the experiment if the random force is neglected. Neglecting the random force is an even more severe approximation than freezing the positions of the metal atoms or modelling the lattice vibrations as a generalized Langevin oscillator. This behavior can be understood by considering analytic solutions to the Ornstein-Uhlenbeck process, where a ballistic particle experiencing friction decelerates under the influence of thermal fluctuations.
- Published
- 2021
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