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Ab initio quantum direct dynamics simulations of ultrafast photochemistry with Multiconfigurational Ehrenfest approach
Chemical Physics ( IF 2.3 ) Pub Date : 2017-04-14 00:00:00 , DOI: 10.1016/j.chemphys.2017.04.003
Dmitry V. Makhov , Christopher Symonds , Sebastian Fernandez-Alberti , Dmitrii V. Shalashilin

The Multiconfigurational Ehrenfest (MCE) method is a quantum dynamics technique which allows treatment of a large number of quantum nuclear degrees of freedom. This paper presents a review of MCE and its recent applications, providing a summary of the formalisms, including its ab initio direct dynamics versions and also giving a summary of recent results. Firstly, we describe the Multiconfigurational Ehrenfest version 2 (MCEv2) method and its applicability to direct dynamics and report new calculations which show that the approach converges to the exact result in model systems with tens of degrees of freedom. Secondly, we review previous “on the fly” ab initio Multiple Cloning (AIMC-MCE) MCE dynamics results obtained for systems of a similar size, in which the calculations treat every electron and every nucleus of a polyatomic molecule on a fully quantum basis. We also review the Time Dependent Diabatic Basis (TDDB) version of the technique and give an example of its application. We summarise the details of the sampling techniques and interpolations used for calculation of the matrix elements, which make our approach efficient. Future directions of work are outlined.

中文翻译:

b从头与Multiconfigurational爱伦菲斯特方法超快光化学量子直接动力学模拟

多构Ehrenfest(MCE)方法是一种量子动力学技术,可以处理大量的量子核自由度。本文介绍了MCE及其最近的应用,提供了形式主义的摘要,包括从头开始的直接动力学版本,还提供了最新结果的摘要。首先,我们描述了多配置Ehrenfest版本2(MCEv2)方法及其在指导动力学方面的适用性,并报告了新的计算结果,这些结果表明该方法收敛于具有数十个自由度的模型系统中的精确结果。其次,我们回顾先前的“动态”从头算对于相似大小的系统,获得了多克隆(AIMC-MCE)MCE动力学结果,其中计算在完全量子的基础上处理了多原子分子的每个电子和每个核。我们还将回顾该技术的时间依赖绝热基础(TDDB)版本,并给出其应用示例。我们总结了用于矩阵元素计算的采样技术和插值的细节,这使我们的方法有效。概述了未来的工作方向。
更新日期:2017-06-27
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