Efficient and low-scaling linear-response time-dependent density functional theory implementation for core-level spectroscopy of large and periodic systems

Literature Information

Publication Date 2021-02-08
DOI 10.1039/D0CP06164F
Impact Factor 3.676
Authors

Augustin Bussy, Jürg Hutter


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Abstract

We discuss our implementation of linear-response time-dependent density functional theory (LR-TDDFT) for core level near-edge absorption spectroscopy. The method is based on established LR-TDDFT approaches to X-ray absorption spectroscopy (XAS) with additional accurate approximations for increased efficiency. We validate our implementation by reproducing benchmark results at the K-edge and showing that spin–orbit coupling effects at the L2,3-edge are well described. We also demonstrate that the method is suitable for extended systems in periodic boundary conditions and measure a favorable sub-cubic scaling of the calculation cost with system size. We finally show that GPUs can be efficiently exploited and report speedups of up to a factor 2.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
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