Optimal control in a dissipative system: Vibrational excitation of CO/Cu(100) by IR pulses

Stephanie Beyvers, Yukiyoshi Ohtsuki, Peter Saalfrank

Research output: Contribution to journalArticlepeer-review

41 Citations (Scopus)

Abstract

The question as to whether state-selective population of molecular vibrational levels by shaped infrared laser pulses is possible in a condensed phase environment is of central importance for such diverse fields as time-resolved spectroscopy, quantum computing, or "vibrationally mediated chemistry." This question is addressed here for a model system, representing carbon monoxide adsorbed on a Cu(100) surface. Three of the six vibrational modes are considered explicitly, namely, the CO stretch vibration, the CO-surface vibration, and a frustrated translation. Optimized infrared pulses for state-selective excitation of "bright" and "dark" vibrational levels are designed by optimal control theory in the framework of a Markovian open-system density matrix approach, with energy flow to substrate electrons and phonons, phase relaxation, and finite temperature accounted for. The pulses are analyzed by their Husimi "quasiprobability" distribution in time-energy space.

Original languageEnglish
Article number234706
JournalJournal of Chemical Physics
Volume124
Issue number23
DOIs
Publication statusPublished - 2006 Jun 21

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Fingerprint

Dive into the research topics of 'Optimal control in a dissipative system: Vibrational excitation of CO/Cu(100) by IR pulses'. Together they form a unique fingerprint.

Cite this