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J. Phys. Soc. Jpn. 69 (2000) pp. 4095-4106  |Next Article|  |Table of Contents|
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Two-Dimensional Spectroscopy for Harmonic Vibrational Modes with Nonlinear System-Bath Interactions. II. Gaussian-Markovian Case

Yoshitaka Tanimura and Thomas Steffen1

Institute for Molecular Science and the Graduate University for Advanced Studies,
Myodaiji, Okazaki, Aichi 444-8585
1Ultrafast Laser and Spectroscopy Laboratory, Department of Chemical Physics,
University of Groningen, Nijenborgh 4, 9747 AG Groningen, The Netherlands

(Received July 3, 2000)

The relaxation processes in a quantum system nonlinearly coupled to a harmonic Gaussian-Markovian heat bath are investigated by the quantum Fokker-Planck equation in the hierarchy form. This model describes frequency fluctuations in the quantum system with an arbitrary correlation time and thus bridges the gap between the Brownian oscillator model and the stochastic model by Anderson and Kubo. The effects of the finite correlation time and the system-bath coupling strength are studied for a harmonic model system by numerically integrating the equation of motion. The one-time correlation function of the system coordinate, which is measured in conventional Raman and infrared absorption experiments, already reflects the inhomogeneous character of the relaxation process. The finite correlation time of the frequency fluctuations, however, is directly evident only in the two- and three-time correlation function as probed by multidimensional spectroscopic techniques such as the Raman echo and the fifth-order 2D Raman experiment. ©2000 The Physical Society of Japan

URL: http://jpsj.ipap.jp/link?JPSJ/69/4095/
DOI: 10.1143/JPSJ.69.4095


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