Postdoc: A Scalable Parallel Approach to Molecular Dynamics with Quantum Transitions

提出了一种可扩展的并行算法，用于计算具有量子跃迁的分子动力学。分子动力学中包含量子跃迁意味着必须沿着经典原子核的轨迹求解电子自由度的薛定谔方程。由于缺乏对每个绝热波函数的基态膨胀系数导数的具体解析表达式，使得经典原子核上的力的计算变得复杂。这个问题可以用微扰理论来解决，但是得到的方程必须迭代求解。这种迭代计算，以及随后的力和波函数导数的计算可以对每个经典坐标并行进行。概述了该算法在特定化学体系和电子结构方法中的应用。考虑到大量表现出非绝热效应的化学和物理现象，这里概述的算法应该广泛适用。这是并行计算机应用于非绝热动力学的第一个实例。

A scalable parallel algorithm is proposed for carrying out molecular dynamics with quantum transitions. The inclusion of quantum transitions in molecular dynamics implies that one must solve the Schrodinger equation for the electronic degrees of freedom along the trajectory of the classical nuclei. The calculation of forces on the classical nuclei is complicated by the lack of specific analytic expressions for derivatives of the basis state expansion coefficients for each adiabatic wavefunction. The problem can be solved through the use of perturbation theory, however the resulting equations must be solved iteratively. This iterative calculation, and subsequent calculation of forces and wavefunction derivatives can be done in parallel for each classical coordinate. The application of the algorithm to a specific chemical system and electronic structure method is outlined. Given the large number of chemical and physical phenomena that exhibit nonadiabatic effects, the algorithm outlined here should be widely applicable. This proposal represents the first instance of the application of parallel computers to nonadiabatic dynamics.