Development and implementation of modern density functional methods for property calculations

在基于实空间描述的密度泛函理论中，新一代依赖位置和轨道的交换关联泛函将被开发并应用到ARTEN和Turomole量子化学程序中。我们的目标是实现比当前技术状态所表示的更通用和通用的泛函，而不需要广泛的参数化。泛函应该同样适用于热化学、动力学、磁学和电学性质以及激发光谱。发展的主要途径是：a)进一步改进局域杂化泛函的局域混合函数和随后的验证，b)用于大分子激发谱含时密度泛函计算的局域杂化泛函的高效自洽实现，c)将Becke的非动力学关联的实空间模型扩展为计算高效的自洽实现。

New generations of position- and orbital-dependent exchange-correlation functionals in density functional theory based on real-space descriptions shall be developed and implemented into the ReSpect and Turbomole quantum-chemical programs. We aim towards more general and universal functionals than represented by the current state of the art, without extensive parameterization. The functionals should be applicable equally well for thermochemistry, kinetics, magnetic and electric properties as well as excitation spectra. The main routes of development are: a) further improvement of local mixing functions for local hybrid functionals and subsequent validation, b) efficient self-consistent implementation of local hybrid functionals for time-dependent DFT calculations of excitation spectra of large molecules, c) extension of Becke's real-space model for non-dynamical correlation into a computationally efficient self-consistent implementation.