非绝热动力学的激子方法:超越弗伦克尔激子模型

IF 5.7 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Chemical Theory and Computation Pub Date : 2024-09-16 DOI:10.1021/acs.jctc.4c00886
Eduarda Sangiogo Gil, Andrea Giustini, Davide Accomasso, Giovanni Granucci
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引用次数: 0

摘要

我们报告了扩展弗伦克尔激子模型(EFEM)的制定和实施情况,该模型旨在模拟多色团系统的动力学,其中考虑到了可能存在的色团间电荷转移状态以及两种色团同时激发的其他状态。我们的方法包括根据对多色相聚合体中的单体和选定二聚体进行的计算构建哈密顿。非绝热分子动力学采用表面跳跃方法,而构建 EFEM 所需的电子波函数和能量则采用半经验浮动占位分子轨道-配置相互作用(FOMO-CI)电子结构方法计算。为了验证我们的方法,我们模拟了嵌入晶体环境中的 2,5-双(芴-9-亚基)-2,5-二氢噻吩(ThBF)分子三聚体的单子裂变过程,并将 EFEM 的结果与标准 "超级分子 "方法进行了比较。
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Excitonic Approach for Nonadiabatic Dynamics: Extending Beyond the Frenkel Exciton Model
We report the formulation and implementation of an extended Frenkel exciton model (EFEM) designed for simulating the dynamics of multichromophoric systems, taking into account the possible presence of interchromophore charge transfer states, as well as other states in which two chromophores are simultaneously excited. Our approach involves constructing a Hamiltonian based on calculations performed on monomers and selected dimers within the multichromophoric aggregate. Nonadiabatic molecular dynamics is addressed using a surface hopping approach, while the electronic wave functions and energies required for constructing the EFEM are computed utilizing the semiempirical floating occupation molecular orbitals-configuration interaction (FOMO-CI) electronic structure method. To validate our approach, we simulate the singlet fission process in a trimer of 2,5-bis(fluorene-9-ylidene)-2,5-dihydrothiophene (ThBF) molecules, embedded in their crystal environment, comparing the results of the EFEM to the standard “supermolecule” approach.
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来源期刊
Journal of Chemical Theory and Computation
Journal of Chemical Theory and Computation 化学-物理:原子、分子和化学物理
CiteScore
9.90
自引率
16.40%
发文量
568
审稿时长
1 months
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Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere.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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