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

文献情報

出版日 2021-02-08

DOI 10.1039/D0CP06164F

インパクトファクター 3.676

著者

Augustin Bussy, Jürg Hutter

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要旨

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.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.