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• W2059896429 abstract "The correlation between coherent driving and non-Markovian dissipation plays a vital role in optical processes. To exhibit its effect on the simulation of optical spectroscopy, we explore the correlated driving-dissipation equation (CODDE) [R. X. Xu and Y. J. Yan, J. Chem. Phys. 116, 9196 (2002)]10.1063/1.1474579, which modifies the conventional Redfield theory with the inclusion of correlated driving-dissipation effect at the second-order system–bath coupling level. With an exciton model mimicking the Fenna–Matthews–Olson pigment-protein complex, we compare between the Redfield theory, CODDE, and exact hierarchical dynamics, for their results on linear absorption and coherent two-dimensional spectroscopy. We clarify that the failure of Redfield approach originates mainly from the neglect of driving–dissipation correlation, rather than its second-order nature. We further propose a dynamical inhomogeneity parameter to quantify the applicable range of CODDE. Our results indicate that CODDE is an efficient and quantifiable theory for many light-harvesting complexes of interest. To facilitate the evaluation of multi-dimensional spectroscopy, we also develop the mixed Heisenberg–Schrödinger picture scheme that is valid for any dynamics implementation on nonlinear response functions." @default.
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• W2059896429 date "2013-01-10" @default.
• W2059896429 modified "2023-10-16" @default.
• W2059896429 title "Correlated driving and dissipation in two-dimensional spectroscopy" @default.
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• W2059896429 doi "https://doi.org/10.1063/1.4773472" @default.
• W2059896429 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/23320667" @default.
• W2059896429 hasPublicationYear "2013" @default.
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