Coherent Stokes Raman scattering with incoherent light for vibrational-dephasing-time measurement

Toshiaki Hattori, Akira Terasaki, Takayoshi Kobayashi

研究成果: ジャーナルへの寄稿学術誌査読

86 被引用数 (Scopus)


A new method to measure picosecond or subpicosecond vibrational-dephasing dynamics with the use of incoherent or broadband light is presented theoretically and experimentally. It is based on a transient coherent Raman process with three beams. In our experimental scheme, two of them are incoherent light from a single source, and a delay time between the two is variable. A third beam has a higher frequency than the incoherent light by a vibrational energy in a molecule of interest, and is coherent in the delay-time range of the measurement. The delay-time dependence of coherent Stokes Raman scattering (CSRS) intensity offers the information about the coherence dynamics of the vibrational transition with a resolution time determined only by the correlation time of the incoherent light. For the theoretical calculation, a three-level model of the molecular system with homogeneous broadening is used, and delay-time dependences of the CSRS signal are calculated for off-resonance and resonance cases. Dephasing dynamics of the 2915-cm-1 mode in dimethylsulfoxide was observed experimentally by the new method with the use of nanosecond laser pulses, and the result agrees well with that obtained with picosecond pulses.

ジャーナルPhysical Review A
出版ステータス出版済み - 1987

!!!All Science Journal Classification (ASJC) codes

  • 原子分子物理学および光学


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