A CLASSICAL-MODEL FOR TIME-RESOLVED AND FREQUENCY-RESOLVED SPECTROSCOPY OF NONADIABATIC EXCITED-STATE DYNAMICS

被引：25

作者：

STOCK, G ^{[1
]}

MILLER, WH ^{[1
]}

机构：

[1] UNIV CALIF BERKELEY, DEPT CHEM, BERKELEY, CA 94720 USA

来源：

CHEMICAL PHYSICS LETTERS | 1992年 / 197卷 / 4-5期

关键词：

D O I：

10.1016/0009-2614(92)85791-8

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Based on the framework of the classical electron analog due to Meyer and Miller, we outline a new classical formulation of the spectroscopy of nonadiabatically coupled electronic states. The time-dependent molecular correlation functions are expressed in terms of the classical dipole function that is the classical analog of the quantum-mechanical electronic dipole operator. Explicit expressions for cw absorption and for time- and frequency-resolved pump-probe spectra are derived. The capability of the classical method is illustrated by computational results for a four-mode model of the S2-S1 conical intersection in pyrazine. Comparison to exact quantum-mechanical calculations reveals that the classical model reproduces the qualitative features of the cw absorption and the time- and frequency-resolved spectra.

引用

页码：396 / 404

页数：9

共 59 条

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