STATISTICAL ASPECTS OF THE RADIATIVE EXCITATION OF THE HARMONIC-OSCILLATOR

Citation
R. Marquardt et M. Quack, STATISTICAL ASPECTS OF THE RADIATIVE EXCITATION OF THE HARMONIC-OSCILLATOR, Journal of physical chemistry, 98(13), 1994, pp. 3486-3491
Citations number
68
Categorie Soggetti
Chemistry Physical
ISSN journal
00223654
Volume
98
Issue
13
Year of publication
1994
Pages
3486 - 3491
Database
ISI
SICI code
0022-3654(1994)98:13<3486:SAOTRE>2.0.ZU;2-G
Abstract
We report solutions of the master equation for infrared multiphoton ex citation of a harmonic oscillator with linear dipole function in a the rmal radiation field (including spontaneous emission). The time-depend ent populations and wave packet motions are discussed in comparison to coherent laser excitation and in relation to quantum ''chaotic'' moti on arising from random phases in a perfectly regular spectrum. A Loren tzian envelope for high overtone line strength distributions arising f rom hypothetical highly nonlinear dipole functions of the harmonic osc illator allows one to reconstruct a Bixon-Jortner-like model with a si mple one-dimensional harmonic oscillator. Numerical simulation of cohe rent radiative resonance overtone excitation shows Rabi oscillation co rresponding to an effective two-level model. Short-pulse excitation pr epares a superposition state which thereafter decays. This decay corre sponds to a simple one-dimensional motion of an initially displaced wa ve packet, with the expected recurrence at the oscillator period, but without substantial intermediate spreading of probability.