Ultrafast coherent dynamics of nonadiabatically coupled quasi-degenerate excited states in molecules: Population and vibrational coherence transfers

H. Mineo, Manabu Kanno, Hirohiko Kono, S. D. Chao, S. H. Lin, Y. Fujimura

Research output: Contribution to journalArticlepeer-review

10 Citations (Scopus)

Abstract

Results of a theoretical study of ultrafast coherent dynamics of nonadiabatically coupled quasi-degenerate π-electronic excited states of molecules were presented. Analytical expressions for temporal behaviors of population and vibrational coherence were derived using a simplified model to clarify the quantum mechanical interferences between the two coherently excited electronic states, which appeared in the nuclear wavepacket simulations [M. Kanno, H. Kono, Y. Fujimura, S.H. Lin, Phys. Rev. Lett 104 (2010) 108302]. The photon-polarization direction of the linearly polarized laser, which controls the populations of the two quasi-degenerate electronic states, determines constructive or destructive interference. Features of the vibrational coherence transfer between the two coupled quasi-electronic states through nonadiabatic couplings are also presented. Information on both the transition frequency and nonadiabatic coupling matrix element between the two states can be obtained by analyzing signals of two kinds of quantum beats before and after transfer through nonadiabatic coupling.

Original languageEnglish
Pages (from-to)136-142
Number of pages7
JournalChemical Physics
Volume392
Issue number1
DOIs
Publication statusPublished - 2012 Jan 2

Keywords

  • Nonadiabatically coupled quasi-degenerate states
  • Pi electron rotations
  • Population transfer
  • Quantum beats
  • Quantum mechanical interference
  • Ultrafast coherent dynamics
  • Vibrational coherence transfer

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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