Multiconfigurational Ehrenfest approach to quantum coherent dynamics in large molecular systems.
Multiconfigurational Ehrenfest approach to quantum coherent dynamics in large molecular systems.
复制标题
大分子系统中量子相干动力学的多配置埃伦费斯特方法。
DOI：
10.1039/c1fd00034a
复制
发表时间：
2011
影响因子：
3.4
通讯作者：
D. Shalashilin
中科院分区：
文献类型：
--
作者：
D. Shalashilin
本文简要介绍了最近开发的多配置 Ehrenfest 动力学方法，用于模拟多自由度系统中的量子动力学。中心思想是通过埃伦菲斯特轨迹来引导基波函数的轨迹。引导基函数的幅度通过线性方程组耦合。该方法已应用于自旋玻色子模型和吡嗪分子中的非绝热动力学模拟。报道了吡嗪 24D 模型中非绝热动力学的新应用，其中仅基于 34 基 Ehrenfest 配置就获得了良好的光谱。该应用为未来的全量子直接动力学奠定了基础。系统浴哈密顿量描述的粘着表面模型的另一个新应用被提出，以证明该方法的广泛性，该方法可应用于电子绝热和非绝热动力学。对于所有应用，结果与 MCTDH 的结果非常一致，这是其他基于轨迹的方法很难实现的。因此，MCE 可以作为未来使用“即时”直接动力的起点。 MCE 提供了一种有效的全量子方法，能够捕获多维系统中的相干动力学，这是开发和理解现实量子系统中相干控制的必要步骤。
This article briefly describes recently developed Multiconfigurational Ehrenfest dynamics method to simulate quantum dynamics in systems with many degrees of freedom. The central idea is to guide the trajectories of basis wave functions by means of the Ehrenfest trajectories. The amplitudes of guided basis functions are coupled through a system of linear equations. The approach has been applied to simulations of nonadiabatic dynamics in Spin-Boson model and in pyrazine molecule. A new application to nonadiabatic dynamics in 24D model of pyrazine, where good spectrum for is obtained with the basis of only 34 basis Ehrenfest configurations is reported. This application provides the ground for future fully quantum direct dynamics. Another new application to the model of sticking to the surface described by the System-Bath Hamiltonian is presented to demonstrate the broadness of the approach, which can be applied to both electronically adiabatic and nonadiabatic dynamics. For all applications the results are in good agreement with those of MCTDH, which is very difficult to achieve with other trajectory-based methods. Therefore MCE can serve as a starting point for future use with "on the fly" direct dynamics. MCE provides an efficient fully quantum method capable of catching coherent dynamics in multidimentional systems, which is a necessary step for developing and understanding coherent control in realistic quantum systems.
影响因子：
4.4
作者：
Burghardt, I.;Giri, K.;Worth, G. A.
通讯作者：
Worth, G. A.