Department of Physics and Astronomy , Hunter College and the Graduate Center of the City University of New York , 695 Park Avenue , New York , New York 10065 , United States.
J Chem Theory Comput. 2019 Mar 12;15(3):1672-1678. doi: 10.1021/acs.jctc.8b01159. Epub 2019 Feb 14.
We present a new class of nonadiabatic approximations in time-dependent density functional theory derived from an exact expression for the time-dependent exchange-correlation potential. The approximations reproduce dynamical step and peak features in the exact potential that are missing in adiabatic approximations. Central to this approach is an approximation for the one-body reduced density-matrix as a functional of the Kohn-Sham density-matrix, and we examine the performance of two such approximations on four examples.
我们提出了一类新的非绝热时间相关密度泛函理论近似，该近似源于时间相关交换关联势的精确表达式。该近似能够再现动力学阶跃和峰特征，而这些特征在绝热近似中是缺失的。该方法的核心是将单粒子约化密度矩阵作为 Kohn-Sham 密度矩阵的泛函进行近似，我们在四个示例上检验了两种此类近似的性能。
