Journal
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
Volume 16, Issue 2, Pages 1064-1072Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jctc.9b01121
Keywords
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Funding
- National Science Foundation [DMR-1828019, DMR-1922042, CHE-1763176]
- Department of Energy, Photonics at Thermodynamic Limits Energy Frontier Research Center [DE-SC0019140]
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Generalized Kohn-Sham density functional theory is a popular computational tool for the ground state of extended systems, particularly within range-separated hybrid (RSH) functionals that capture the long-range electronic interaction. Unfortunately, the heavy computational cost of the nonlocal exchange operator in RSH-DFT usually confines the approach to systems with at most a few hundred electrons. A significant reduction in the computational cost is achieved by representing the density matrix with stochastic orbitals and a stochastic decomposition of the Coulomb convolution (J. Phys. Chem. A 2016, 120, 3071). Here, we extend the stochastic RSH approach to excited states within the framework of linear-response generalized Kohn-Sham time-dependent density functional theory (GKS-TDDFT) based on the plane-wave basis. As a validation of the stochastic GKS-TDDFT method, the excitation energies of small molecules N-2 and CO are calculated and compared to the deterministic results. The computational efficiency of the stochastic method is demonstrated with a two-dimensional MoS2 sheet (1500 electrons), whose excitation energy, exciton charge density, and (excited state) geometric relaxation are determined in the absence and presence of a point defect.
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