Open AccessRandom Force in Molecular Dynamics with Electronic Friction
Author(s) -
Nils Hertl,
Raidel Martin-Barrios,
Oihana Galparsoro,
P. Larrégaray,
Daniel J. Auerbach,
Dirk Schwarzer,
Alec M. Wodtke,
Alexander Kandratsenka
Publication year - 2021
Publication title -
journal of physical chemistry. c./journal of physical chemistry. c
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.401
H-Index - 289
eISSN - 1932-7455
pISSN - 1932-7447
DOI - 10.1021/acs.jpcc.1c03436
Subject(s) - langevin equation , brownian motion , physics , thermal fluctuations , molecular dynamics , langevin dynamics , classical mechanics , statistical physics , brownian dynamics , conservative force , thermal , diffusion , quantum mechanics , thermodynamics
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.