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Title: Non-Markovian response of ultrafast coherent electronic ring currents in chiral aromatic molecules in a condensed phase

Results of a theoretical study on non-Markov response for femtosecond laser-driven coherent ring currents in chiral aromatic molecules embedded in a condensed phase are presented. Coherent ring currents are generated by coherent excitation of a pair of quasi-degenerated π-electronic excited states. The coherent electronic dynamical behaviors are strongly influenced by interactions between the electronic system and phonon bath in a condensed phase. Here, the bath correlation time is not instantaneous but should be taken to be a finite time in ultrashort time-resolved experiments. In such a case, Markov approximation breaks down. A hierarchical master equation approach for an improved semiclassical Drude dissipation model was adopted to examine the non-Markov effects on ultrafast coherent electronic ring currents of (P)-2,2{sup ′}-biphenol in a condensed phase. Time evolution of the coherent ring current derived in the hierarchical master equation approach was calculated and compared with those in the Drude model in the Markov approximation and in the static limit. The results show how non-Markovian behaviors in quantum beat signals of ring currents depend on the Drude bath damping constant. Effects of temperatures on ultrafast coherent electronic ring currents are also clarified.
Authors:
 [1] ;  [1] ;  [2] ;  [1] ;  [3] ;  [4] ;  [5] ;  [6] ;  [7] ;  [2]
  1. Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan (China)
  2. (China)
  3. (Japan)
  4. Department of Chemistry, Nankai University, Tianjin 300071 (China)
  5. (Hong Kong)
  6. Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026 (China)
  7. Department of Chemistry, Hong Kong University of Science and Technology, Kowloon (Hong Kong)
Publication Date:
OSTI Identifier:
22251288
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 139; Journal Issue: 21; Other Information: (c) 2013 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 97 MATHEMATICAL METHODS AND COMPUTING; CHIRALITY; EQUATIONS; EXCITED STATES; INTERACTIONS; MARKOV PROCESS; MOLECULES; RING CURRENTS; SEMICLASSICAL APPROXIMATION