论文标题
用固定状态的耦合群集群集多电子动力学的解释
Interpretation of Coupled-Cluster Many-Electron Dynamics in Terms of Stationary States
论文作者
论文摘要
我们从理论上和数字上证明了激光驱动的多电子动力学,如双性时间依赖性耦合群集理论所描述的那样,可以根据固定态群体进行分析。通过线性响应理论和动作方程耦合群集理论来定义的投影仪,提出了与激光脉冲或其他外部力量相互作用期间的固态种群的计算,并讨论了人群的保护定律。拟议投影仪的数值测试,包括He和Be Atoms的线性和非线性光学过程,以及对于Lih,Ch $^+$和LIF分子的数值测试,表明,在整个站点上,在所有阶段都非常接近的是完整的coustration countion(CCSD)级别的固定态人群的激光驱动的演变(ccsd)级别,这些级别是完整的。在动力学中,足够近似。当双激发状态对于动力学很重要时,CCSD结果的质量会恶化。观察到从线性响应投影仪计算的种群可能显示出虚假的小型振幅,高频振荡,运动方程投影仪是作为固定态种群的最有希望的方法而出现的。
We demonstrate theoretically and numerically that laser-driven many-electron dynamics, as described by bivariational time-dependent coupled-cluster theory, may be analyzed in terms of stationary-state populations. Projectors heuristically defined from linear response theory and equation-of-motion coupled-cluster theory are proposed for the calculation of stationary-state populations during interaction with laser pulses or other external forces, and conservation laws of the populations are discussed. Numerical tests of the proposed projectors, involving both linear and nonlinear optical processes for the He and Be atoms, and for the LiH, CH$^+$, and LiF molecules, show that the laser-driven evolution of the stationary-state populations at the coupled-cluster singles-and-doubles (CCSD) level is very close to that obtained by full configuration-interaction theory provided all stationary states actively participating in the dynamics are sufficiently well approximated. When double-excited states are important for the dynamics, the quality of the CCSD results deteriorate. Observing that populations computed from the linear-response projector may show spurious small-amplitude, high-frequency oscillations, the equation-of-motion projector emerges as the most promising approach to stationary-state populations.