NON-MARKOVIAN OPTICAL DEPHASING DYNAMICS IN ROOM-TEMPERATURE LIQUIDS INVESTIGATED BY FEMTOSECOND TRANSIENT ABSORPTION-SPECTROSCOPY - THEORY AND EXPERIMENT

被引：79

作者：

CONG, PJ ^{[1
]}

YAN, YJ ^{[1
]}

DEUEL, HP ^{[1
]}

SIMON, JD ^{[1
]}

机构：

[1] UNIV CALIF SAN DIEGO, INST NONLINEAR SCI, LA JOLLA, CA 92093 USA

来源：

JOURNAL OF CHEMICAL PHYSICS | 1994年 / 100卷 / 11期

关键词：

D O I：

10.1063/1.466832

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：

This paper examines the electronic dephasing dynamics of the dye molecule HITCI in an ethylene glycol solution. Degenerate transient absorption data are presented as a function of laser pulse width and detuning from the absorption maximum. The dephasing dynamics revealed by the experimental results are shown to be non-Markovian. The experimental data cannot be quantitatively described by stochastic theories that assume a single relaxation time for the solvent. A model is presented that includes contributions from both fast and slow modulations to the absorption line shape. Using this approach, quantitative agreement is observed between theory and experiment. These results clearly indicate that multiple time scales for liquid dynamics contribute to the absorption line shape of solute molecules. The solvent parameters obtained are discussed in light of results from complementary experiments designed to measure characteristic relaxation times:

引用

页码：7855 / 7866

页数：12

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