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首页> 外文期刊>The Journal of Chemical Physics >Efficient rel-space configuration-interaction method for te simulation of multielectron mixed quantum and classicla nonadiabatic molecular dynamics in the condensed phase
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Efficient rel-space configuration-interaction method for te simulation of multielectron mixed quantum and classicla nonadiabatic molecular dynamics in the condensed phase

机译：凝聚相中多电子混合量子和经典非绝热分子动力学的有效rel-space配置-相互作用方法

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摘要

We introduce an efficient configuration interaction(CI) mehtod for the calculation of mixed quantum and classical nonadiabatic molecular dynamics for multiple electrons.For any given realization of the classical degrees of freedom(e.g.,a solvent),the method uses a novel real-space quadrature to efficiently compute the Coulomb and exchange interactions between electrons.We also introduce an approximation whereby the classical molecular dynamics is propageated for several time steps on electronic potential energy surfaces generated using only a particularly important subset of the CI basis states.By only updating the important-states subset periodically,we achieve significant reductions in the computational cost of solving the multielectron quantum problem.We test the real-space quadrature for the cases of two electrons confined in a cubic box with infinitely repulsive walls and two electrons dissolved in liquid water that occupy a single cavity,so-called hydrated dielectrons.We then demonstrate how to perform mixed quantum and classical nonadiabatic dynamics by combinin ghtese computational techniques iwth the mean-field with surface hopping algorithm of Prezhdo and Rossky[J.Chem.Phys.107,825(1997)].Finally,we illustrate the practicality of the approach to multielectron nonadiabatic dynamcs by examining the nonadiabatic relaxation dynamics of both spin singlet and spin triplet hydrated dielectrons following excitation from the ground to the first excited state.
机译：我们介绍了一种有效的构型相互作用（CI）方法，用于计算多个电子的混合量子和经典非绝热分子动力学。对于经典自由度的任何给定实现（例如溶剂），该方法均使用新颖的实空间正交以有效地计算库仑和电子之间的相互作用。我们还引入了一种近似方法，其中经典分子动力学在仅使用CI重要基态的一个特别重要子集生成的电子势能面上进行了几个时间步的传播。重要周期子集，我们大大降低了解决多电子量子问题的计算量。我们测试了两个电子在一个无限排斥壁的立方盒中以及两个电子溶解在液态水中的情况下的实空间正交性占据一个空腔的水合双电子结合Prezhdo和Rossky的表面跳变算法，结合平均场与平均场的计算技术，阐述了如何执行混合量子和经典非绝热动力学[J.Chem.Phys.107,825（1997）]。最后，我们说明了该方法的实用性通过检查自基态激发到第一激发态后自旋单重态和自旋三重态水合双电子的非绝热弛豫动力学，得到多电子非绝热动力学。

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