Electron-transfer-induced dissociation of H2 on gold nanoparticles: Excited-state potential energy surfaces via embedded correlated wavefunction theory

Florian Libisch, Jin Cheng, Emily A. Carter

Research output: Contribution to journalArticle

29 Scopus citations

Abstract

Noble metal surfaces play a central role in heterogeneous catalysis. Lasers of the appropriate resonance frequency efficiently generate surface plasmons. These, in turn, may generate hot electrons, which can drive catalytic reactions at low temperatures. In this work, we demonstrate how embedding methods allow for the use of accurate ab-initio correlated wavefunction methods to describe excited-state potential energy surfaces of molecule-surface interactions. As model system, we consider the hot-electron-induced dissociation of hydrogen on Au(111), which has recently been demonstrated experimentally. We discuss merits and limitations of several different correlated wavefunction schemes. Our results show that dissociation barriers may be substantially reduced upon electron excitation and suggest a method to calculate the hot electron energies required for catalytic reactions.

Original languageEnglish (US)
Pages (from-to)1455-1466
Number of pages12
JournalZeitschrift fur Physikalische Chemie
Volume227
Issue number11
DOIs
StatePublished - Nov 1 2013

All Science Journal Classification (ASJC) codes

  • Physical and Theoretical Chemistry

Keywords

  • Photocatalysis
  • Plasmons
  • Potential Energy Surfaces

Fingerprint Dive into the research topics of 'Electron-transfer-induced dissociation of H<sub>2</sub> on gold nanoparticles: Excited-state potential energy surfaces via embedded correlated wavefunction theory'. Together they form a unique fingerprint.

  • Cite this