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Title: Efficient simulation of time- and frequency-resolved four-wave-mixing signals with a multiconfigurational Ehrenfest approach
Authors: Chen, Lipeng
Sun, Kewei
Shalashilin, Dmitrii V.
Gelin, Maxim F.
Zhao, Yang
Keywords: Engineering::Materials
Issue Date: 2021
Source: Chen, L., Sun, K., Shalashilin, D. V., Gelin, M. F. & Zhao, Y. (2021). Efficient simulation of time- and frequency-resolved four-wave-mixing signals with a multiconfigurational Ehrenfest approach. Journal of Chemical Physics, 154(5), 054105-.
Project: 2018-T1-002-175
MOE2019- T2-1-085
Journal: Journal of Chemical Physics
Abstract: We have extended the multiconfigurational Ehrenfest approach to the simulation of four-wave-mixing signals of systems involving multiple electronic and vibrational degrees of freedom. As an illustration, we calculate signals of three widely used spectroscopic techniques, time- and frequency-resolved fluorescence spectroscopy, transient absorption spectroscopy, and two-dimensional (2D) electronic spectroscopy, for a two-electronic-state, twenty-four vibrational-mode conical intersection model. It has been shown that all these three spectroscopic signals characterize fast population transfer from the higher excited electronic state to the lower excited electronic state. While the time- and frequency-resolved spectrum maps the wave packet propagation exclusively on the electronically excited states, the transient absorption and 2D electronic spectra reflect the wave packet dynamics on both electronically excited states and the electronic ground state. Combining trajectory-guided Gaussian basis functions and the nonlinear response function formalism, the present approach provides a promising general technique for the applications of various Gaussian basis methods to the calculations of four-wave-mixing spectra of polyatomic molecules.
ISSN: 0021-9606
DOI: 10.1063/5.0038824
Rights: © 2021 Author(s). All rights reserved. This paper was published by AIP Publishing in Journal of Chemical Physics and is made available with permission of Author(s).
Fulltext Permission: open
Fulltext Availability: With Fulltext
Appears in Collections:MSE Journal Articles

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