Christov Ivan P
Department of Physics, Sofia University, 1164 Sofia, Bulgaria.
J Chem Phys. 2008 Dec 7;129(21):214107. doi: 10.1063/1.3031214.
In this paper we propose an ab initio method to solve quantum many-body problems of molecular dynamics where both electronic and nuclear degrees are represented by ensembles of trajectories and guiding waves in physical space. Both electrons and nuclei can be treated quantum mechanically where the guiding waves obey a set of coupled Schrodinger equations (quantum-quantum description) or, alternatively, coupled Schrodinger-Newtonian equations are solved for the quantum-classical approximation. The method takes into account local and nonlocal quantum correlation effects in a self-consistent manner. The general formalism is applied to one- and two-dimensional hydrogen molecules subjected to a strong ultrashort optical pulse. Comparison is made with the results from the "exact" Ehrenfest molecular dynamics for the molecular ionization and for the evolution of the internuclear distance as the molecule dissociates.
在本文中，我们提出了一种从头算方法来解决分子动力学中的量子多体问题，其中电子和核自由度都由物理空间中的轨迹系综和引导波来表示。电子和核都可以用量子力学方法处理，其中引导波服从一组耦合的薛定谔方程（量子-量子描述），或者，也可以求解耦合的薛定谔-牛顿方程以进行量子-经典近似。该方法以自洽的方式考虑了局部和非局部量子相关效应。将一般形式体系应用于受到强超短光脉冲作用的一维和二维氢分子。将结果与“精确”的埃伦费斯特分子动力学对于分子电离以及分子解离时核间距演化的结果进行了比较。
