2013年12月
Simulation of femtosecond "double-slit" experiments for a chromophore in a dissipative environment
JOURNAL OF CHEMICAL PHYSICS
- ,
- ,
- 巻
- 139
- 号
- 21
- 開始ページ
- 214302
- 終了ページ
- 記述言語
- 英語
- 掲載種別
- 研究論文(学術雑誌)
- DOI
- 10.1063/1.4832876
- 出版者・発行元
- AMER INST PHYSICS
We performed simulations of the prototypical femtosecond "double-slit" experiment with strong pulsed laser fields for a chromophore in solution. The chromophore is modeled as a system with two electronic levels and a single Franck-Condon active underdamped vibrational mode. All other (intra- and inter-molecular) vibrational modes are accounted for as a thermal bath. The system-bath coupling is treated in a computationally accurate manner using the hierarchy equations of motion approach. The double-slit signal is evaluated numerically exactly without invoking perturbation theory in the matter-field interaction. We show that the strong-pulse double-slit signal consists of a superposition of N-wave-mixing (N = 2, 4, 6...) responses and can be split into population and coherence contributions. The former reveals the dynamics of vibrational wave packets in the ground state and the excited electronic state of the chromophore, while the latter contains information on the dephasing of electronic coherences of the chromophore density matrix. We studied the influence of heat baths with different coupling strengths and memories on the double-slit signal. Our results show that the double-slit experiment performed with strong (nonperturbative) pulses yields substantially more information on the photoinduced dynamics of the chromophore than the weak-pulse experiment, in particular, if the bath-induced dephasings are fast. (C) 2013 AIP Publishing LLC.
- リンク情報
- ID情報
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- DOI : 10.1063/1.4832876
- ISSN : 0021-9606
- eISSN : 1089-7690
- Web of Science ID : WOS:000328636400020