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激子模型中的表面跳跃。一种静电嵌入方案。

Surface Hopping within an Exciton Picture. An Electrostatic Embedding Scheme.

作者信息

Menger Maximilian F S J, Plasser Felix, Mennucci Benedetta, González Leticia

机构信息

Institute for Theoretical Chemistry, Faculty of Chemistry , University of Vienna , Währingerstrasse 17 , 1090 Vienna , Austria.

Dipartimento di Chimica e Chimica Industriale , University of Pisa , Via G. Moruzzi 13 , 56124 Pisa , Italy.

出版信息

J Chem Theory Comput. 2018 Dec 11;14(12):6139-6148. doi: 10.1021/acs.jctc.8b00763. Epub 2018 Nov 6.

DOI:10.1021/acs.jctc.8b00763
PMID:30299941
Abstract

We report the development and the implementation of an exciton approach that allows ab initio nonadiabatic dynamics simulations of electronic excitation energy transfer in multichromophoric systems. For the dynamics, a trajectory-based strategy is used within the surface hopping formulation. The approach features a consistent hybrid formulation that allows the construction of potential energy surfaces and gradients by combining quantum mechanics and molecular mechanics within an electrostatic embedding scheme. As an application, the study of a molecular dyad consisting of a covalently bound BODIPY moiety and a tetrathiophene group is presented using time-dependent density functional theory (TDDFT). The results obtained with the exciton model are compared to previously performed full TDDFT dynamics of the same system. Our results show excellent agreement with the full TDDFT results, indicating that the couplings that lead to excitation energy transfer (EET) are dominated by Coulomb interaction terms and that charge-transfer states are not necessary to properly describe the nonadiabatic dynamics of the system. The exciton model also reveals ultrafast coherent oscillations of the excitation between the two units in the dyad, which occur during the first 50 fs.

摘要

我们报告了一种激子方法的开发与实施,该方法能够对多发色团体系中的电子激发能量转移进行从头算非绝热动力学模拟。对于动力学过程,在表面跳跃公式内采用基于轨迹的策略。该方法具有一致的混合公式,通过在静电嵌入方案中结合量子力学和分子力学来构建势能面和梯度。作为应用,使用含时密度泛函理论(TDDFT)对由共价连接的硼二吡咯部分和四噻吩基团组成的分子二元体系进行了研究。将激子模型得到的结果与该体系先前进行的全TDDFT动力学结果进行了比较。我们的结果与全TDDFT结果显示出极好的一致性,表明导致激发能量转移(EET)的耦合主要由库仑相互作用项主导,并且电荷转移态对于正确描述该体系的非绝热动力学并非必要。激子模型还揭示了二元体系中两个单元之间激发的超快相干振荡,这种振荡发生在最初的50飞秒内。

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