Theoretische Physik IV, Universität Bayreuth, D-95440 Bayreuth, Germany.
J Chem Phys. 2012 Aug 14;137(6):064117. doi: 10.1063/1.4742763.
We present a real-time Kohn-Sham propagation scheme for the self-interaction correction (SIC). The multiplicative Kohn-Sham potential is constructed in real-time and real-space based on the generalized optimized effective potential equation. We demonstrate that this approach yields promising results for a wide range of test systems, including hydrogen terminated silicon clusters, conjugated molecular chains, and molecular charge-transfer systems. We analyze the nature of excitations by calculating transition densities from the time evolution and by evaluating the time-dependent exchange-correlation potential. A properly constructed Kohn-Sham SIC potential shows a time-dependent field-counteracting behavior. These favorable characteristics of the exchange-correlation potential may be lost in approximations such as the SIC-Slater potential.
我们提出了一种用于自相互作用校正（SIC）的实时 Kohn-Sham 传播方案。基于广义优化有效势方程，在实时和实空间中构建乘法 Kohn-Sham 势。我们证明了这种方法对于广泛的测试系统，包括氢终止硅团簇、共轭分子链和分子电荷转移系统，都能产生有前景的结果。我们通过计算从时间演化得出的跃迁密度和评估时变交换相关势，来分析激发的性质。适当构造的 Kohn-Sham SIC 势表现出与时间相关的场抵消行为。这些交换相关势的有利特性可能会在 SIC-Slater 势等近似中丢失。
