Mapping of Wave Packet Dynamics at Conical Intersections by Time- and Frequency-Resolved Fluorescence Spectroscopy: A Computational Study

被引：24

作者：

Chen, Lipeng ^{[1
]}

Gelin, Maxim F. ^{[1
]}

Zhao, Yang ^{[2
]}

Domcke, Wolfgang ^{[1
]}

机构：

[1] Tech Univ Munich, Dept Chem, D-85747 Garching, Germany

[2] Nanyang Technol Univ, Div Mat Sci, 50 Nanyang Ave, Singapore 639798, Singapore

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2019年 / 10卷 / 19期

关键词：

HIERARCHY EQUATIONS; MOLECULAR-DYNAMICS; QUANTUM DYNAMICS; PHOTOISOMERIZATION; RELAXATION; PHOTOCHEMISTRY; SIMULATIONS; PYRAZINE; MOTION; PHASE;

D O I：

10.1021/acs.jpclett.9b02208

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：

Monitoring of wave packet dynamics at conical intersections by time- and frequency-resolved fluorescence spectroscopy has been investigated theoretically for a three-state two-mode model of a conical intersection coupled to a dissipative environment. The ideal and the actually measurable time- and frequency-gated fluorescence spectra are accurately and efficiently simulated by combining the hierarchy equations-of-motion method for dissipative quantum dynamics with the methodology of the equation-of-motion phase-matching approach for the calculation of spectroscopic signals. It is shown that time- and frequency-resolved fluorescence spectra reveal essential aspects of the wave packet dynamics at conical intersections and the effects of environment-induced dissipation. The results of the present work indicate that fluorescence up-conversion spectroscopy with femtosecond time resolution is an efficient tool for the characterization of ultrafast dynamics at conical intersections.

引用

页码：5873 / 5880

页数：8

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