期刊
CHEMICAL PHYSICS
卷 404, 期 -, 页码 103-115出版社
ELSEVIER
DOI: 10.1016/j.chemphys.2012.02.022
关键词
Non-linear optical response; Open quantum systems; Projection operator techniques
资金
- Czech Science Foundation (GACR) grant [205/10/0989]
- Ministry of Education, Youth and Sports of the Czech Republic [KONTAKT ME899]
- [GAUK 416311]
We demonstrate the application of the recently introduced parametric projector operator technique to a calculation of the second order non-linear optical response of a multilevel molecular system. We derive a parametric quantum master equation (QME) for the time evolution of the excited state of an excitonic system after excitation by the first two pulses in the usual spectroscopic four-wave-mixing scheme. This master equation differs from the usual QME by a correction term which depends on the delay tau between the pulses. In the presence of environmental degrees of freedom with finite bath correlation time and in the presence of intramolecular vibrations we find distinct dynamics of both the excited state populations and the electronic coherence for different delays tau. (C) 2012 Elsevier B.V. All rights reserved.
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