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arXiv · 2402.16217

Sparse-Stochastic Fragmented Exchange for Large-Scale Hybrid TDDFT Calculations

Mykola Sereda·Tucker Allen·Nadine C. Bradbury·Khaled Z. Ibrahim·Daniel Neuhauser
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Abstract

We extend our recently developed sparse-stochastic fragmented exchange formalism for ground-state hybrid DFT (ngH-DFT) to calculate absorption spectra within linear-response time-dependent Generalized Kohn-Sham DFT (LR-GKS-TDDFT), for systems consisting of thousands of valence electrons within a grid-based/plane-wave representation. A mixed deterministic/fragmented-stochastic compression of the exchange kernel, here using long-range explicit exchange functionals, provides an efficient method for accurate optical spectra. Both real-time propagation as well frequency-resolved Casida-equation-type approaches for spectra are presented, and the method is applied to large molecular dyes.

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Mykola Sereda, Tucker Allen, Nadine C. Bradbury, Khaled Z. Ibrahim, Daniel Neuhauser. 2024-02-25. Sparse-Stochastic Fragmented Exchange for Large-Scale Hybrid TDDFT Calculations. https://doi.org/10.1021/acs.jctc.4c00260

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