Origin of Power Laws for Reactions at Metal Surfaces Mediated by Hot Electrons

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Abstract

A wide range of experiments have established that certain chemical reactions at metal surfaces can be driven by multiple hot-electron-mediated excitations of adsorbates. A high transient density of hot electrons is obtained by means of femtosecond laser pulses and a characteristic feature of such experiments is the emergence of a power law dependence of the reaction yield on the laser fluence Y similar to F-n. We propose a model of multiple inelastic scattering by hot electrons which reproduces this power law and the observed exponents of several experiments. All parameters are calculated within density functional theory and the delta self-consistent field method. With a simplifying assumption, the power law becomes exact and we obtain a simple physical interpretation of the exponent n, which represents the number of adsorbate vibrational states participating in the reaction.
Original languageEnglish
JournalPhysical Review Letters
Volume103
Issue number23
Pages (from-to)238301
ISSN0031-9007
DOIs
Publication statusPublished - 2009

Bibliographical note

Copyright 2009 American Physical Society

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