Modeling vibrational dephasing and energy relaxation of intramolecular anharmonic modes for multidimensional infrared spectroscopies
Open accessAbstract
Starting from a system-bath Hamiltonian in a molecular coordinate representation, we examine an applicability of a stochastic multilevel model for vibrational dephasing and energy relaxation in multidimensional infrared spectroscopy. We consider an intramolecular anharmonic mode nonlinearly coupled to a colored noise bath at finite temperature. The system-bath interaction is assumed linear plus square in the system coordinate, but linear in the bath coordinates. The square-linear system-bath interaction leads to dephasing due to the frequency fluctuation of system vibration, while the linear-linear interaction contributes to energy relaxation and a part of dephasing arises from anharmonicity. To clarify the role and origin of vibrational dephasing and energy relaxation in the stochastic model, the system part is then transformed into an energy eigenstate representation without using the rotating wave approximation. Two-dimensional (2D) infrared spectra are then calculated by solving a low-temperature corrected quantum Fokker-Planck (LTC-QFP) equation for a colored noise bath and by the stochastic theory. In motional narrowing regime, the spectra from the stochastic model are quite different from those from the LTC-QFP. In spectral diffusion regime, however, the 2D line shapes from the stochastic model resemble those from the LTC-QFP besides the blueshifts caused by the dissipation from the colored noise bath. The preconditions for validity of the stochastic theory for molecular vibrational motion are also discussed.
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The hierarchy equation method provides an exact treatment of decoherence and employs neither the rotating-wave, Born, nor Markovian approximations.
“The set of hierarchy equations derived here provides an exact treatment of decoherence, and employs neither the rotating-wave, Born, nor Markovian approximations.”
From Quantum speed limits in open systems: Non-Markovian dynamics without rotating-wave approximation (2015) · cites this paper as [23]
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“(23) is extended over all time intervals (ai, bi) in which g is positive, and the maximum is taken over all pairs of initial states.”
Background
- Authors
- Ishizaki, A., & Tanimura, Y.
- Affiliations
- Kyoto University (JP)
- Venue
- The Journal of Chemical Physics
- Publisher
- AIP Publishing
- Published
- 2006-08-22
- Volume
- 125
- Issue
- 8
- Pages
- 084501-084501
- ISSN
- 0021-9606 (ISSN-L)
- 1089-7690
- OpenAlex
- W2001507797
- Cited by
- 115
- References
- 86
- Citations by year
- 2026: 4 · 2025: 3 · 2023: 4 · 2022: 4 · 2021: 4 · 2020: 6 · 2019: 6 · 2018: 3 · 2017: 8 · 2016: 4 · 2015: 12 · 2014: 8 · 2013: 4 · 2012: 9
- FWCI
- 5.38
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Locations
- The Journal of Chemical Physics (publishedVersion)
- PubMed (publishedVersion)
- Institutional Repositories DataBase (IRDB) (submittedVersion)
- Kyoto University Research Information Repository (Kyoto University) (submittedVersion)
- Funders
- Japan Society for the Promotion of Science (15205005)
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Physical Sciences › Chemistry › Spectroscopy › Spectroscopy and Laser Applications
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Biophysics › Spectroscopy Techniques in Biomedical and Chemical Research
- Keywords
- vibrational dephasing, energy relaxation, motional narrowing, spectral diffusion, anharmonicity, frequency variation
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