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.
@article{arxiv.2402.16217,
title = {Sparse-Stochastic Fragmented Exchange for Large-Scale Hybrid TDDFT Calculations},
author = {Mykola Sereda and Tucker Allen and Nadine C. Bradbury and Khaled Z. Ibrahim and Daniel Neuhauser},
journal= {arXiv preprint arXiv:2402.16217},
year = {2025}
}
Comments
22 pages, 4 figures. First two authors are equal contributors to this work and designated as co-first authors