TY - JOUR
T1 - Electron-transfer-induced dissociation of H2 on gold nanoparticles
T2 - Excited-state potential energy surfaces via embedded correlated wavefunction theory
AU - Libisch, Florian
AU - Cheng, Jin
AU - Carter, Emily A.
N1 - Funding Information:
We thank C. Huang, G. Kresse, S. Mukherjee, and P. Nordlander for valuable discussions. We gratefully acknowledge support from the Office of Naval Research and the National Science Foundation. Calculations were performed on the CSES high performance computing cluster at Princeton University, and on the Vienna Scientific Cluster.
PY - 2013/11
Y1 - 2013/11
N2 - 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.
AB - 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.
KW - Photocatalysis
KW - Plasmons
KW - Potential Energy Surfaces
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U2 - 10.1524/zpch.2013.0406
DO - 10.1524/zpch.2013.0406
M3 - Article
AN - SCOPUS:84888606210
SN - 0942-9352
VL - 227
SP - 1455
EP - 1466
JO - Zeitschrift fur Physikalische Chemie
JF - Zeitschrift fur Physikalische Chemie
IS - 11
ER -