TY - JOUR
T1 - Optical-heterodyne-detected induced phase modulation for the study of femtosecond molecular dynamics
AU - Hattori, Toshiaki
AU - Terasaki, Akira
AU - Kobayashi, Takayoshi
AU - Wada, Tatsuo
AU - Yamada, Akira
AU - Sasabe, Hiroyuki
PY - 1991/1/1
Y1 - 1991/1/1
N2 - A new experimental technique for the study of ultrafast optical response of nonlinear materials, which detects nonrelaxational response in the media with high sensitivity, is introduced. Polarization-selective optical-heterodyne- detection scheme is applied to the measurement of the spectral shift of a probe pulse which is caused by induced phase modulation (IPM) brought about by a pump pulse. This technique, being sensitive to the high-frequency component of the nonlinear response, is especially applicable to the study of intermolecular dynamics in disordered media. The temporal responses of the optical Kerr effect in liquid carbon tetrachloride, benzene, and carbon disulfide are studied using this technique with femtosecond optical pulses. In the response of benzene, damped oscillations are clearly observed which are due to intermolecular vibrational motions of the molecules. The data obtained from benzene and carbon disulfide are analyzed using a Fourier-transform method. The response functions for the IPM measurements are reconstructed, and the Fourier spectra are also obtained. They are discussed in terms of inertial molecular motions and the local structures in these liquids.
AB - A new experimental technique for the study of ultrafast optical response of nonlinear materials, which detects nonrelaxational response in the media with high sensitivity, is introduced. Polarization-selective optical-heterodyne- detection scheme is applied to the measurement of the spectral shift of a probe pulse which is caused by induced phase modulation (IPM) brought about by a pump pulse. This technique, being sensitive to the high-frequency component of the nonlinear response, is especially applicable to the study of intermolecular dynamics in disordered media. The temporal responses of the optical Kerr effect in liquid carbon tetrachloride, benzene, and carbon disulfide are studied using this technique with femtosecond optical pulses. In the response of benzene, damped oscillations are clearly observed which are due to intermolecular vibrational motions of the molecules. The data obtained from benzene and carbon disulfide are analyzed using a Fourier-transform method. The response functions for the IPM measurements are reconstructed, and the Fourier spectra are also obtained. They are discussed in terms of inertial molecular motions and the local structures in these liquids.
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U2 - 10.1063/1.461102
DO - 10.1063/1.461102
M3 - Article
AN - SCOPUS:0000400177
VL - 95
SP - 937
EP - 945
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 2
ER -