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Energy Dissipation during Diffusion at Metal Surfaces: Disentangling the Role of Phonons versus Electron-Hole Pairs

Accepted version
Peer-reviewed

Type

Article

Change log

Authors

Rittmeyer, SP 
Ward, DJ 
Gütlein, P 
Ellis, J 
Allison, W 

Abstract

Helium spin echo experiments combined with ab initio based Langevin molecular dynamics simulations are used to quantify the adsorbate-substrate coupling during the thermal diffusion of Na atoms on Cu(111). An analysis of trajectories within the local density friction approximation allows the contribution from electron-hole pair excitations to be separated from the total energy dissipation. Despite the minimal electronic friction coefficient of Na and the relatively small mass mismatch to Cu promoting efficient phononic dissipation, about (20±5)% of the total energy loss is attributable to electronic friction. The results suggest a significant role of electronic nonadiabaticity in the rapid thermalization generally relied upon in adiabatic diffusion theories.

Description

Keywords

0306 Physical Chemistry (incl. Structural)

Journal Title

Physical Review Letters

Conference Name

Journal ISSN

0031-9007
1079-7114

Volume Title

117

Publisher

American Physical Society
Sponsorship
Engineering and Physical Sciences Research Council (EP/E004962/1)
S. P. R. acknowledges the support of the Technische Universität München—Institute for Advanced Study, funded by the German Excellence Initiative and the European Union Seventh Framework Programme under Grant Agreement No. 291763.