Recent advances and perspectives in four-component Dirac-Kohn-Sham calculations
Recent advances and perspectives in four-component Dirac-Kohn-Sham calculations
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DOI：
10.1039/c1cp20569b
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发表时间：
2011-01-01
影响因子：
3.3
通讯作者：
Tarantelli, Francesco
中科院分区：
文献类型：
--
作者：
Belpassi, Leonardo;Storchi, Loriano;Tarantelli, Francesco
本文综述了全相对论四组分Dirac-Kohn-Sham （DKS）方法在计算含有许多重原子的化学体系的电子结构方面的最新理论和计算进展。我们描述了基于g旋量基集、埃尔米特高斯函数、最先进的密度拟合技术和内存分布式并行性的全电子DKS方法的实现。这种方法极大地扩展了DKS方法的适用性，包括例如大型重原子簇，并为未来的关键发展开辟了道路。我们研究了DKS方法目前的局限性和未来可能的应用，包括四电流密度泛函和实时传播方案的实现。这将使描述强场中的分子成为可能，准确地解释相对论运动效应和自旋轨道耦合。
We review recent theoretical and computational advances in the full relativistic four-component Dirac-Kohn-Sham (DKS) approach and its application to the calculation of the electronic structure of chemical systems containing many heavy atoms. We describe our implementation of an all-electron DKS approach based on the use of G-spinor basis sets, Hermite Gaussian functions, state-of-the-art density-fitting techniques and memory distributed parallelism. This approach has enormously extended the applicability of the DKS method, including for example large clusters of heavy atoms, and opens the way for future key developments. We examine the current limitations and future possible applications of the DKS approach, including the implementation of four-current density functionals and real-time propagation schemes. This would make possible to describe molecules in strong fields, accurately accounting for relativistic kinematic effects and spin-orbit coupling.