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記事

84 引用 (Scopus)

抄録

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.

元の言語英語
ページ(範囲)715-724
ページ数10
ジャーナルPhysical Review A
35
発行部数2
DOI
出版物ステータス出版済み - 1 1 1987
外部発表Yes

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time measurement
Raman spectra
time dependence
time lag
picosecond pulses
broadband
pulses
lasers
molecules
energy

All Science Journal Classification (ASJC) codes

  • Atomic and Molecular Physics, and Optics

これを引用

Coherent Stokes Raman scattering with incoherent light for vibrational-dephasing-time measurement. / Hattori, Toshiaki; Terasaki, Akira; Kobayashi, Takayoshi.

:: Physical Review A, 巻 35, 番号 2, 01.01.1987, p. 715-724.

研究成果: ジャーナルへの寄稿記事

Hattori, Toshiaki ; Terasaki, Akira ; Kobayashi, Takayoshi. / Coherent Stokes Raman scattering with incoherent light for vibrational-dephasing-time measurement. :: Physical Review A. 1987 ; 巻 35, 番号 2. pp. 715-724.
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abstract = "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.",
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N2 - 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.

AB - 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.

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