Photodesorption of NO from a metal surface: Quantum dynamical implications of a two-mode model

Peter Saalfrank; Gisela Boendgen; Karin Finger; Lorenzo Luigi Pesce

doi:10.1016/S0301-0104(99)00314-6

Photodesorption of NO from a metal surface: Quantum dynamical implications of a two-mode model

Peter Saalfrank, Gisela Boendgen, Karin Finger, Lorenzo Luigi Pesce

Pharmacology

Research output: Contribution to journal › Article › peer-review

31 Scopus citations

Abstract

Open-system density matrix theory is used to study the dissipative quantum dynamics of photoinduced, hot-electron mediated desorption of NO from Pt(111). Two electronic states are considered and both the DIET (Desorption Induced by Electronic Transitions) and DIMET (Desorption Induced by Multiple Electronic Transitions) limits addressed. Besides the center-of-mass motion of the molecule perpendicular to the surface plane, the vibrational motion of the NO molecule is accounted for. In a first, methodological part the interrelations between various "direct" and "jumping wave packet" methods to solve the underlying open-system Liouville-von Neumann equations of motion, are emphasized. In a second, applied part we investigate (i) the relevance of the popular "negative ion resonance" model, (ii) the role of coordinate-dependent electronic relaxation, and (iii) the implications of multiple-electronic excitations.

Original language	English (US)
Pages (from-to)	51-69
Number of pages	19
Journal	Chemical Physics
Volume	251
Issue number	1-3
DOIs	https://doi.org/10.1016/S0301-0104(99)00314-6
State	Published - Jan 1 2000

Funding

We thank H. Guo (Albuquerque) and J. Manz (Berlin) for stimulating discussions. Generous support by the Deutsche Forschungsgemeinschaft (“Schwerpunktprogramm Zeitabhängige Phänomene und Methoden in Quantensystemen der Physik und Chemie”, project-no. Sa 547/2, now Ma 515/17) is gratefully acknowledged.

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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Cite this

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title = "Photodesorption of NO from a metal surface: Quantum dynamical implications of a two-mode model",

abstract = "Open-system density matrix theory is used to study the dissipative quantum dynamics of photoinduced, hot-electron mediated desorption of NO from Pt(111). Two electronic states are considered and both the DIET (Desorption Induced by Electronic Transitions) and DIMET (Desorption Induced by Multiple Electronic Transitions) limits addressed. Besides the center-of-mass motion of the molecule perpendicular to the surface plane, the vibrational motion of the NO molecule is accounted for. In a first, methodological part the interrelations between various {"}direct{"} and {"}jumping wave packet{"} methods to solve the underlying open-system Liouville-von Neumann equations of motion, are emphasized. In a second, applied part we investigate (i) the relevance of the popular {"}negative ion resonance{"} model, (ii) the role of coordinate-dependent electronic relaxation, and (iii) the implications of multiple-electronic excitations.",

author = "Peter Saalfrank and Gisela Boendgen and Karin Finger and Pesce, {Lorenzo Luigi}",

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AU - Saalfrank, Peter

AU - Boendgen, Gisela

AU - Finger, Karin

AU - Pesce, Lorenzo Luigi

N1 - Funding Information: We thank H. Guo (Albuquerque) and J. Manz (Berlin) for stimulating discussions. Generous support by the Deutsche Forschungsgemeinschaft (“Schwerpunktprogramm Zeitabhängige Phänomene und Methoden in Quantensystemen der Physik und Chemie”, project-no. Sa 547/2, now Ma 515/17) is gratefully acknowledged.

PY - 2000/1/1

Y1 - 2000/1/1

N2 - Open-system density matrix theory is used to study the dissipative quantum dynamics of photoinduced, hot-electron mediated desorption of NO from Pt(111). Two electronic states are considered and both the DIET (Desorption Induced by Electronic Transitions) and DIMET (Desorption Induced by Multiple Electronic Transitions) limits addressed. Besides the center-of-mass motion of the molecule perpendicular to the surface plane, the vibrational motion of the NO molecule is accounted for. In a first, methodological part the interrelations between various "direct" and "jumping wave packet" methods to solve the underlying open-system Liouville-von Neumann equations of motion, are emphasized. In a second, applied part we investigate (i) the relevance of the popular "negative ion resonance" model, (ii) the role of coordinate-dependent electronic relaxation, and (iii) the implications of multiple-electronic excitations.

AB - Open-system density matrix theory is used to study the dissipative quantum dynamics of photoinduced, hot-electron mediated desorption of NO from Pt(111). Two electronic states are considered and both the DIET (Desorption Induced by Electronic Transitions) and DIMET (Desorption Induced by Multiple Electronic Transitions) limits addressed. Besides the center-of-mass motion of the molecule perpendicular to the surface plane, the vibrational motion of the NO molecule is accounted for. In a first, methodological part the interrelations between various "direct" and "jumping wave packet" methods to solve the underlying open-system Liouville-von Neumann equations of motion, are emphasized. In a second, applied part we investigate (i) the relevance of the popular "negative ion resonance" model, (ii) the role of coordinate-dependent electronic relaxation, and (iii) the implications of multiple-electronic excitations.

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Photodesorption of NO from a metal surface: Quantum dynamical implications of a two-mode model

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