| Project/Area Number |
08640657
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| Research Category |
Grant-in-Aid for Scientific Research (C)
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| Allocation Type | Single-year Grants |
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| Section | 一般 |
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| Research Field |
Physical chemistry
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| Research Institution | Okazaki National Resarch Institute |
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Principal Investigator |
TANIMURA Yoshitaka Okazaki National Resarch Institute, Institute for Molecular Science, 分子科学研究所, 助教授 (20270465)
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| Co-Investigator(Kenkyū-buntansha) |
OKUMURA Ko Okazaki National Resarch Institute, Institute for Molecular Science, Institute f, 分子科学研究所, 助手 (80271500)
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| Project Period (FY) |
1996 – 1997
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| Project Status |
Completed (Fiscal Year 1997)
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| Budget Amount *help |
¥1,000,000 (Direct Cost: ¥1,000,000)
Fiscal Year 1997: ¥1,000,000 (Direct Cost: ¥1,000,000)
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| Keywords | 2D Raman / Path Integral / Fokker-Planck / Femto-second / nonlinear optics / Brownian / 非調和振動子 / 経路積分 / CS_2 |
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| Research Abstract |
The nonlinear optical response of a molecular system in the condensed phase subjected to a series of off-resonant femtosecond laser pulses has been studied to investigate inhomogeneous broadening of liquid states and anharmonicity of vibrational modes. We have derived analytical expressions of the 5th order response function for an anharmonic system using path-integral techniques. Applying this equation, we have studied the interplay between anharmonicity and inhomogeneity. The fifth-order response function for a displaced anharmonic system has been also derived and applied to study photon echo, pump-probe experiments and newly developed the fifth-order experiment which is designed to detect weak anharmonicity of potentials.
Using a quantum Fokker-Planck equation, we have studied higher-order optical processes of Morse potential systems. This Fokker-Planck equation can treat a molecular system with any shape of potential coupled to a Gaussian-white or a Gaussian Markovian noise-bath. We
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have presented a procedure to calculate the third-and fifth-order response functions, which are equivalent to the second-and third-order correlation functions of the molecular coordinate, by way of the eq. of motion approach. Assuming the potential surface of a Cesium dimer, which is modeled by the Morse potential, and the linear and nonlinear coordinate dependence of the polarizability, we calculated the third-and fifth-order response functions for various temperatures and heat-bath couplings. By plotting two time-evolution period involved in the fifth-order spectroscopy, we obtained the two-dimensional profiles of the signals. These 2D profiles are sensitive for a shape of potential and polarizability, even for a strong damping case, and depend on the temperature. This indicates that fifth-order two-dimensional spectroscopy carried out for a different temperature allows us to access information of the potential and the polarizability. We have also presented the Fokker-Planck equation for multi-state systems and applied to the displaced Morse oscillators system. Optical Stark effects of it was observed and discussed. Less
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