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Quasi-Diabatic Representation for Nonadiabatic Dynamics Propagation
Journal of Chemical Theory and Computation ( IF 5.5 ) Pub Date : 2018-02-28 00:00:00 , DOI: 10.1021/acs.jctc.7b01178
Arkajit Mandal 1 , Sharma SRKC Yamijala 1 , Pengfei Huo 1
Affiliation  

We develop a nonadiabatic dynamics propagation scheme that allows interfacing diabatic quantum dynamics methods with commonly used adiabatic electronic structure calculations. This scheme uses adiabatic states as the quasi-diabatic (QD) states during a short-time quantum dynamics propagation. At every dynamical propagation step, these QD states are updated based on a new set of adiabatic basis. Using the partial linearized density matrix (PLDM) path-integral method as one specific example for diabatic dynamics approaches, we demonstrate the accuracy of the QD scheme with a wide range of model nonadiabatic systems as well as the on-the-fly propagations with density functional tight-binding (DFTB) calculations. This study opens the possibility to combine accurate diabatic quantum dynamics methods with adiabatic electronic structure calculations for nonadiabatic dynamics propagations.

中文翻译:

非绝热动力学传播的拟绝热表示

我们开发了一种非绝热动力学传播方案,该方案允许将绝热量子动力学方法与常用的绝热电子结构计算接口。该方案在短时量子动力学传播过程中将绝热状态用作准绝热(QD)状态。在每个动态传播步骤,这些QD状态都基于一组新的绝热基础进行更新。使用部分线性化密度矩阵(PLDM)路径积分方法作为非绝热动力学方法的一个特定示例,我们证明了QD方案在各种模型非绝热系统中的精确度以及具有密度的实时传播功能紧密绑定(DFTB)计算。
更新日期:2018-02-28
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