Two-Dimensional Spectroscopy for Harmonic Vibrational Modes with Nonlinear System-Bath Interactions. I. Gaussian-White Case.

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  • Steffen Thomas
    Ultrafast Laser and Spectroscopy Laboratory, Department of Chemical Physics, University of Groningen, Nijenborgh 4, 9747 AG Groningen, The Netherlands
  • Tanimura Yoshitaka
    Institute for Molecular Science and the Graduate University for Advanced Studies, Myodaiji, Okazaki, Aichi 444–8585

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  • Two-Dimensional Spectroscopy for Harmonic Vibrational Modes with Nonlinear System-Bath Interactions(1)Gaussian-White Case

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The quantum Fokker-Planck equation is derived for a system nonlinearly coupled to a harmonic oscillator bath. The system-bath interaction is assumed to be linear in the bath coordinates but quadratic in the system coordinate. The relaxation induced dynamics of a harmonic system are investigated by simulating the higher-order correlation functions of the Raman polarizability and the dipole moment, which represent the nonlinear optical responses of Raman or infrared spectroscopy. The 5th-order Raman response shows that, in addition to the frequency fluctuations induced by the bath, higher-order energy transfer between the system and bath plays a role. The nonlinearity of the system-bath interaction yields also an interesting feature in the 7th-order Raman echo or the 3rd-order infrared photon echo response: The calculations predict a finite signal for the case of a harmonic potential and a linear coordinate dependence of the polarizability or dipole while for linear system-bath coupling this response vanishes completely due to destructive interference of different Liouville space pathways.

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