期刊
JOURNAL OF CHEMICAL PHYSICS
卷 140, 期 7, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.4864759
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资金
- (U.S.) Air Force Office of Scientific Research (USAFOSR) [FA9550-13-1-0005]
The response of an arbitrary closed quantum system to a partially coherent electric field is investigated, with a focus on the transient coherences in the system. As a model we examine, both perturbatively and numerically, the coherences induced in a three level V system. Both rapid turn-on and pulsed turn-on effects are investigated. The effect of a long and incoherent pulse is also considered, demonstrating that during the pulse the system shows a coherent response which reduces after the pulse is over. Both the pulsed scenario and the thermally broadened CW case approach a mixed state in the long time limit, with rates dictated by the adjacent level spacings and the coherence time of the light, and via a mechanism that is distinctly different from traditional decoherence. These two excitation scenarios are also explored for a minimal toy model of the electronic levels in pigment protein complex PC645 by both a collisionally broadened CW laser and by a noisy pulse, where unexpectedly long transient coherence times are observed and explained. The significance of environmentally induced decoherence is noted. (C) 2014 AIP Publishing LLC.
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