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Non-adiabatic Couplings in Surface Hopping with Tight Binding Density Functional Theory: The Case of Molecular Motors

表面跳跃 背景(考古学) 密度泛函理论 从头算 放松(心理学) 绝热过程 分子动力学 计算机科学 电子结构 振动耦合 紧密结合 含时密度泛函理论 统计物理学 物理 化学 计算化学 分子 量子力学 心理学 古生物学 社会心理学 生物
作者
Gonzalo Díaz Mirón,Carlos R. Lien-Medrano,Debarshi Banerjee,Marta Monti,Bálint Aradi,Michael A. Sentef,Thomas A. Niehaus,Ali Hassanali
出处
期刊:Journal of Chemical Theory and Computation [American Chemical Society]
标识
DOI:10.1021/acs.jctc.4c01263
摘要

Nonadiabatic molecular dynamics (NAMD) has become an essential computational technique for studying the photophysical relaxation of molecular systems after light absorption. These phenomena require approximations that go beyond the Born-Oppenheimer approximation, and the accuracy of the results heavily depends on the electronic structure theory employed. Sophisticated electronic methods, however, make these techniques computationally expensive, even for medium size systems. Consequently, simulations are often performed on simplified models to interpret the experimental results. In this context, a variety of techniques have been developed to perform NAMD using approximate methods, particularly density functional tight binding (DFTB). Despite the use of these techniques on large systems, where ab initio methods are computationally prohibitive, a comprehensive validation has been lacking. In this work, we present a new implementation of trajectory surface hopping combined with DFTB, utilizing nonadiabatic coupling vectors. We selected the methaniminium cation and furan systems for validation, providing an exhaustive comparison with the higher-level electronic structure methods. As a case study, we simulated a system from the class of molecular motors, which has been extensively studied experimentally but remains challenging to simulate with ab initio methods due to its inherent complexity. Our approach effectively captures the key photophysical mechanism of dihedral rotation after the absorption of light. Additionally, we successfully reproduced the transition from the bright to dark states observed in the time-dependent fluorescence experiments, providing valuable insights into this critical part of the photophysical behavior in molecular motors.
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