期刊
ANNUAL REVIEW OF PHYSICAL CHEMISTRY, VOL 72
卷 72, 期 -, 页码 165-188出版社
ANNUAL REVIEWS
DOI: 10.1146/annurev-physchem-090419-051350
关键词
Franck-Condon; ensemble; cumulant; nonlinear spectroscopy; 2DES
资金
- U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0019053]
- CTC program [DE-SC0020203]
- National Science Foundation [CHE-1955656]
- U.S. Department of Energy (DOE) [DE-SC0020203] Funding Source: U.S. Department of Energy (DOE)
Including both environmental and vibronic effects is crucial for accurate simulation of optical spectra. Two approaches are outlined in the study, one based on static snapshots of chromophore-environment configurations and the other on dynamic excitation energies for time-correlated snapshots. Both approaches show significant potential for advancing accurate optical spectroscopy simulations of complex condensed phase systems.
Including both environmental and vibronic effects is important for accurate simulation of optical spectra, but combining these effects remains computationally challenging. We outline two approaches that consider both the explicit atomistic environment and the vibronic transitions. Both phenomena are responsible for spectral shapes in linear spectroscopy and the electronic evolution measured in nonlinear spectroscopy. The first approach utilizes snapshots of chromophore-environment configurations for which chromophore normal modes are determined. We outline various approximations for this static approach that assumes harmonic potentials and ignores dynamic system-environment coupling. The second approach obtains excitation energies for a series of time-correlated snapshots. This dynamic approach relies on the accurate truncation of the cumulant expansion but treats the dynamics of the chromophore and the environment on equal footing. Both approaches show significant potential for making strides toward more accurate optical spectroscopy simulations of complex condensed phase systems.
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