Abstract

A quantum statistical theory for a laser-driven anharmonic oscillator coupled to a system of many degrees of freedom by means of energy- and phase-dissipative mechanisms is presented. The theory is applied to the description of vibrational dynamics in an admolecule-surface system that are associated with desorption–dissociation processes. It is found that phase relaxation plays an important role in assisting the laser driving force to overcome the anharmonicity and/or detuning bottleneck. It is also shown that a shorter duration of the laser pulse is more efficient for depositing photon energy into the admolecule system.

© 1985 Optical Society of America

Infrared free-electron laser as a probe of vibrational dynamics on surfaces

N. J. Tro, D. A. Arthur, and S. M. George
J. Opt. Soc. Am. B 6(5) 995-1002 (1989)

Theory of photodesorption by infrared-laser–adsorbate coupling

H. J. Kreuzer, Z. W. Gortel, and P. Piercy
J. Opt. Soc. Am. B 4(2) 248-254 (1987)

Ultrafast vibrational energy transfer in the real world: laser ablation, energetic solids, and hemeproteins

Dana D. Dlott
J. Opt. Soc. Am. B 7(8) 1638-1652 (1990)

Theory of laser-stimulated desorption spectroscopy

S. H. Lin, A. Boeglin, and B. Fain
J. Opt. Soc. Am. B 4(2) 211-218 (1987)

Molecular velocities in laser-induced vibrational predesorption

J. Heidberg and D. Hoge
J. Opt. Soc. Am. B 4(2) 242-247 (1987)