Görling Andreas
Lehrstuhl für Theoretische Chemie, Universität Erlangen-Nürnberg, Egerlandstrasse 3, D-91058 Erlangen, Germany.
J Chem Phys. 2005 Aug 8;123(6):62203. doi: 10.1063/1.1904583.
Shortcomings of present density-functional methods are considered. Kohn-Sham and time-dependent density-functional methods using orbital- and state-dependent functionals for exchange-correlation energies, potentials, and kernels are discussed as possible remedy for some of these shortcomings. A view on the Kohn-Sham formalism is presented which differs somewhat from the one conventionally taken. The crucial step of constructing local multiplicative exchange-correlation potentials in Kohn-Sham methods based on orbital- and state-dependent functionals is discussed. The description of open-shell systems via a symmetrized Kohn-Sham formalism employing state-dependent exchange-correlation functionals is elucidated. The generalized adiabatic connection Kohn-Sham approach for the self-consistent treatment of excited states within a density-functional framework is considered. In the latter approach orbital- and state-dependent exchange-correlation functionals occur in a density-functional framework which is no longer based on the Hohenberg-Kohn theorem but on a more general relation between electron densities and local multiplicative potentials.
本文讨论了当前密度泛函方法的不足之处。使用依赖于轨道和状态的泛函来描述交换关联能、势和核的Kohn-Sham方法以及含时密度泛函方法，被视为弥补其中一些不足的可能方法。文中给出了一种对Kohn-Sham形式体系的观点，该观点与传统观点略有不同。讨论了在基于依赖于轨道和状态的泛函的Kohn-Sham方法中构建局部乘法交换关联势的关键步骤。阐明了通过采用依赖于状态的交换关联泛函的对称化Kohn-Sham形式体系对开壳层体系的描述。考虑了在密度泛函框架内对激发态进行自洽处理的广义绝热连接Kohn-Sham方法。在后一种方法中，依赖于轨道和状态的交换关联泛函出现在一个密度泛函框架中，该框架不再基于Hohenberg-Kohn定理，而是基于电子密度与局部乘法势之间更一般的关系。
