A Review on Ab Initio Approaches for Multielectron Dynamics
A Review on Ab Initio Approaches for Multielectron Dynamics
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DOI：
10.1109/jstqe.2015.2438827
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发表时间：
2015-04
影响因子：
4.9
通讯作者：
K. Ishikawa;Takeshi Sato
中科院分区：
文献类型：
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作者：
K. Ishikawa;Takeshi Sato
随着飞秒和阿秒激光以及自由电子激光技术的发展，各种理论方法已经发展到描述原子、分子、团簇和固体在这些激光脉冲作用下的行为。在这里，我们回顾了主要的从头算波函数为基础的数值方法来模拟多电子动力学的原子和分子驱动的强烈的长波长和/或超短短波长激光脉冲。含时薛定谔方程的直接解，尽管其适用性仅限于He，H2和Li，但可以提供精确的描述，并且极大地促进了对动态电子-电子关联的理解。多组态自洽场（MCSCF）方法提供了一个灵活的框架，从该框架可以导出各种方法来处理原子和分子，并有可能系统地控制精度。最近导出了一般MCSCF分子的组态相互作用系数和分子轨道的运动方程。R矩阵理论最初是为研究电子与原子碰撞而发展起来的，它的含时扩展可以真实而精确地描述激光驱动的复杂多电子原子。
In parallel with the evolution of femtosecond and attosecond laser as well as free-electron laser technology, a variety of theoretical methods have been developed to describe the behavior of atoms, molecules, clusters, and solids under the action of those laser pulses. Here, we review major ab initio wave-function-based numerical approaches to simulate multielectron dynamics in atoms and molecules driven by intense long-wavelength and/or ultrashort short-wavelength laser pulses. Direct solution of the time-dependent Schrödinger equation, though its applicability is limited to He, H2, and Li, can provide an exact description and has been greatly contributing to the understanding of dynamical electron-electron correlation. Multiconfiguration self-consistent-field (MCSCF) approach offers a flexible framework from which a variety of methods can be derived to treat both atoms and molecules, with possibility to systematically control the accuracy. The equations of motion of configuration interaction coefficients and molecular orbitals for general MCSCF ansatz have recently been derived. Time-dependent extension of the R-matrix theory, originally developed for electron-atom collision, can realistically and accurately describe laser-driven complex multielectron atoms.