Ultrafast coherent dynamics of nonadiabatically coupled quasi-degenerate excited states in molecules: Population and vibrational coherence transfers |
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Authors: | H MineoM Kanno H KonoSD Chao SH Lin Y Fujimura |
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Institution: | a Institute of Applied Mechanics, National Taiwan University, Taipei 106, Taiwan b Department of Chemistry, Graduate School of Science, Tohoku University, Sendai 980-8578, Japan c Institute of Atomic and Molecular Science, Academia Sinica, Taipei 106, Taiwan d Department of Applied Chemistry, Chiao-Tung University, Hsin-Chu 300, Taiwan |
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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. |
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Keywords: | Ultrafast coherent dynamics Nonadiabatically coupled quasi-degenerate states Population transfer Vibrational coherence transfer Quantum mechanical interference Quantum beats Pi electron rotations |
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