Xiao Wang, Kewei Sun, Haomin Xiao, Yang Zhao and Maxim F. Gelin*,
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引用次数: 0
Abstract
We use the numerically accurate multiple Davydov ansatz with thermo-field dynamics (mDA-TFD) methodology to simulate quantum evolution of the conical intersection (CI)-driven singlet fission (SF) system strongly coupled to an optical cavity. We comprehensively analyze the impact of temperature, cavity-mode frequencies and lifetimes, vibrational coupling, and averaged numbers of photons pumped into the cavity modes on the SF dynamics. We have unveiled several new mechanisms regulating the CI-driven SF process in optical cavities, providing theoretical guidance for enhancing the SF efficiency. In particular, we have demonstrated that the simultaneous variation of several parameters governing SF can cause unconventional but robust cooperative effects, which may help to control SF in real systems.
期刊介绍：
The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
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