論文

査読有り
2013年12月

Simulation of femtosecond "double-slit" experiments for a chromophore in a dissipative environment

JOURNAL OF CHEMICAL PHYSICS
  • M. F. Gelin
  • ,
  • Y. Tanimura
  • ,
  • W. Domcke

139
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
DOI
https://doi.org/10.1063/1.4832876
Web of Science
https://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcAuth=JSTA_CEL&SrcApp=J_Gate_JST&DestLinkType=FullRecord&KeyUT=WOS:000328636400020&DestApp=WOS_CPL
ID情報
  • DOI : 10.1063/1.4832876
  • ISSN : 0021-9606
  • eISSN : 1089-7690
  • Web of Science ID : WOS:000328636400020

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