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 |
| 巻 | 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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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
}
TY - JOUR
T1 - Coherent Stokes Raman scattering with incoherent light for vibrational-dephasing-time measurement
AU - Hattori, Toshiaki
AU - Terasaki, Akira
AU - Kobayashi, Takayoshi
PY - 1987/1/1
Y1 - 1987/1/1
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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U2 - 10.1103/PhysRevA.35.715
DO - 10.1103/PhysRevA.35.715
M3 - Article
AN - SCOPUS:0000573943
VL - 35
SP - 715
EP - 724
JO - Physical Review A
JF - Physical Review A
SN - 2469-9926
IS - 2
ER -