On the density matrix based approach to time-dependent density functional response theory
On the density matrix based approach to time-dependent density functional response theory
复制标题
DOI：
10.1063/1.1353585
复制
发表时间：
2001-04-08
影响因子：
4.4
通讯作者：
Furche, F
中科院分区：
文献类型：
--
作者：
Furche, F
详细分析了基于非相互作用单粒子密度矩阵的时变 Kohn-Sham (TDKS) 响应理论的公式。提出了从 TDKS 单粒子密度矩阵的冯诺依曼型运动方程开始的透明推导。由此产生的方案结构简单，并且可以得到频率相关响应特性的紧凑表达式。从频率相关密度矩阵响应的极点分析推断出激发态的系统处理。建立了激发能的变分原理。通过分析导数技术，激发态性质很简单。该理论为线性缩放实现提供了一个特别合适的起点。磁光特性（例如旋转强度和旋转色散）可从 TDKS 电流密度响应中获得。形式主义是规范不变的。推导了绝热近似 (AA) 内的各种新求和规则。结果表明，基于密度矩阵的公式中不存在激发态的“分配问题”；基于共同密度的方法作为特例包含在内。讨论了 AA 的优点和局限性。 (C) 2001 年美国物理研究所。
The formulation of time-dependent Kohn-Sham (TDKS) response theory based on the noninteracting one-particle density matrix is reanalyzed in detail. A transparent derivation starting from a von-Neumann-type equation of motion for the TDKS one-particle density matrix is presented. The resulting scheme has a simple structure and leads to compact expressions for frequency-dependent response properties. A systematic treatment of excited states is inferred from a pole analysis of the frequency-dependent density matrix response. A variational principle for excitation energies is established. Excited state properties are straightforward by analytical derivative techniques. The theory provides a particularly suitable starting point for linear scaling implementations. Magneto-optic properties such as rotatory strengths and the rotatory dispersion are accessible from the TDKS current-density response. The formalism is gauge-invariant. Various new sum rules within the adiabatic approximation (AA) are derived. It is shown that there is no "assignment problem" for excited states in the density matrix based formulation; the common density based approach is included as a special case. Merits and limitations of the AA are discussed. (C) 2001 American Institute of Physics.