Open-system density matrix description of femtosecond laser desorption of electronically and vibrationally relaxing adsorbates: Single- and two-pulse scenarios

Nest, Mathias and Saalfrank, Peter (2002) Open-system density matrix description of femtosecond laser desorption of electronically and vibrationally relaxing adsorbates: Single- and two-pulse scenarios. JOURNAL OF CHEMICAL PHYSICS, 116 (16). pp. 7189-7199. ISSN 0021-9606, 1089-7690

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Abstract

The femtosecond laser pulse induced desorption of a molecule (NO) from a metal surface (Pt) is investigated by means of open-system density matrix theory. Single- and two-pulse scenarios in the so-called DIMET limit (Desorption Induced by Multiple Electronic Transitions) are considered. Special emphasis is given (a) to a realistic modeling of the temperature profiles of substrate degrees of freedom in response to a laser pulse, (b) to the role of vibrational relaxation of the adsorbate-surface bond, and (c) to a critical comparison of our anharmonic "excitation-deexcitation" approach to the simpler Truncated Harmonic Oscillator model with electronic friction. For the single-pulse case, nonlinear scaling of the desorption yield with laser fluence is demonstrated and found to be in good agreement with experiment. For the two-pulse case, time-resolved correlation diagrams are calculated and interpreted. (C) 2002 American Institute of Physics.

Item Type: Article
Uncontrolled Keywords: DISSIPATIVE QUANTUM DYNAMICS; PHOTON-STIMULATED DESORPTION; DRIVEN SURFACE-REACTIONS; METAL-SURFACES; WAVE-PACKET; MEDIATED PHOTODESORPTION; NO; CO; EXCITATION; PT(111);
Subjects: 500 Science > 540 Chemistry & allied sciences
Divisions: Chemistry and Pharmacy > Institut für Physikalische und Theoretische Chemie
Depositing User: Dr. Gernot Deinzer
Date Deposited: 02 Nov 2021 07:30
Last Modified: 02 Nov 2021 07:30
URI: https://pred.uni-regensburg.de/id/eprint/40378

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