表面跳跃
量子退相干
化学
激子
绝热过程
激发态
统计物理学
化学物理
半经典物理学
极化子
分子动力学
自由度(物理和化学)
物理
量子力学
计算化学
电子
量子
作者
Tammie Nelson,Alexander White,Josiah A. Bjorgaard,Andrew E. Sifain,Yu Zhang,Benjamin Nebgen,Sebastian Fernández-Alberti,Dmitry Mozyrsky,Adrián E. Roitberg,Sergei Tretiak
出处
期刊:Chemical Reviews
[American Chemical Society]
日期:2020-02-10
卷期号:120 (4): 2215-2287
被引量:259
标识
DOI:10.1021/acs.chemrev.9b00447
摘要
Optically active molecular materials, such as organic conjugated polymers and biological systems, are characterized by strong coupling between electronic and vibrational degrees of freedom. Typically, simulations must go beyond the Born–Oppenheimer approximation to account for non-adiabatic coupling between excited states. Indeed, non-adiabatic dynamics is commonly associated with exciton dynamics and photophysics involving charge and energy transfer, as well as exciton dissociation and charge recombination. Understanding the photoinduced dynamics in such materials is vital to providing an accurate description of exciton formation, evolution, and decay. This interdisciplinary field has matured significantly over the past decades. Formulation of new theoretical frameworks, development of more efficient and accurate computational algorithms, and evolution of high-performance computer hardware has extended these simulations to very large molecular systems with hundreds of atoms, including numerous studies of organic semiconductors and biomolecules. In this Review, we will describe recent theoretical advances including treatment of electronic decoherence in surface-hopping methods, the role of solvent effects, trivial unavoided crossings, analysis of data based on transition densities, and efficient computational implementations of these numerical methods. We also emphasize newly developed semiclassical approaches, based on the Gaussian approximation, which retain phase and width information to account for significant decoherence and interference effects while maintaining the high efficiency of surface-hopping approaches. The above developments have been employed to successfully describe photophysics in a variety of molecular materials.
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