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Title: Simulation of time- and frequency-resolved four-wave-mixing signals at finite temperatures: a thermo-field dynamics approach
Authors: Chen, Lipeng
Borrelli, Raffaele
Shalashilin, Dmitrii V.
Zhao, Yang
Gelin, Maxim F.
Keywords: Science::Chemistry
Issue Date: 2021
Source: Chen, L., Borrelli, R., Shalashilin, D. V., Zhao, Y. & Gelin, M. F. (2021). Simulation of time- and frequency-resolved four-wave-mixing signals at finite temperatures: a thermo-field dynamics approach. Journal of Chemical Theory and Computation, 17(7), 4359-4373.
Project: RG 190/18 
RG 87/20 
Journal: Journal of Chemical Theory and Computation 
Abstract: We propose a new approach to simulate four-wave-mixing signals of molecular systems at finite temperatures by combining the multiconfigurational Ehrenfest method with the thermo-field dynamics theory. In our approach, the four-time correlation functions at finite temperatures are mapped onto those at zero temperature in an enlarged Hilbert space with twice the vibrational degrees of freedom. As an illustration, we have simulated three multidimensional spectroscopic signals, time- and frequency-resolved fluorescence spectra, transient-absorption pump-probe spectra, and electronic two-dimensional (2D) spectra at finite temperatures, for a conical intersection-mediated singlet fission model of a rubrene crystal. It is shown that a detailed dynamical picture of the singlet fission process can be extracted from the three spectroscopic signals. An increasing temperature leads to lower intensities of the signals and broadened vibrational peaks, which can be attributed to faster singlet-triplet population transfer and stronger bath-induced electronic dephasing at higher temperatures.
ISSN: 1549-9618
DOI: 10.1021/acs.jctc.1c00259
Schools: School of Materials Science and Engineering 
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Chemical Theory and Computation, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see
Fulltext Permission: open
Fulltext Availability: With Fulltext
Appears in Collections:MSE Journal Articles

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