补充绝热和非绝热方法来理解卟啉衍生物的内部转化动力学

IF 5.5 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Chemical Theory and Computation Pub Date : 2024-12-11 DOI:10.1021/acs.jctc.4c0069810.1021/acs.jctc.4c00698

Pavel S. Rukin, Mariagrazia Fortino, Deborah Prezzi* and Carlo Andrea Rozzi*,

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引用次数: 0

摘要

我们分析了裸卟啉和功能化卟啉在Qy和Qx激发态的内部转换动力学，它们在实验中表现出明显不同的时间常数。通过整合两种互补的方法，即静态计算超模重组能和非绝热分子动力学，我们全面了解了决定两种分子不同行为的因素。我们确定了在激发态之间负责人口转移的关键正常模式和基本模式，并讨论了不同统计和非统计分析在提供基于物理的现象的完整描述方面的功效。

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Complementing Adiabatic and Nonadiabatic Methods To Understand Internal Conversion Dynamics in Porphyrin Derivatives

We analyze the internal conversion dynamics within the Q_y and Q_x excited states of both bare and functionalized porphyrins, which are known to exhibit significantly different time constants experimentally. Through the integration of two complementary approaches, static calculation of per-mode reorganization energies and nonadiabatic molecular dynamics, we achieve a comprehensive understanding of the factors determining the different behavior of the two molecules. We identify the key normal and essential modes responsible for the population transfer between excited states and discuss the efficacy of different statistical and nonstatistical analyses in providing a full physics-based description of the phenomenon.

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来源期刊

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Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere.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.