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Linear-Response Time-Dependent Density Functional Theory with Stochastic Range-Separated Hybrids.
J Chem Theory Comput ; 16(2): 1064-1072, 2020 Feb 11.
Artigo em Inglês | MEDLINE | ID: mdl-31899638
ABSTRACT
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 N2 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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Texto completo: Disponível Coleções: Bases de dados internacionais Base de dados: MEDLINE Idioma: Inglês Revista: J Chem Theory Comput Ano de publicação: 2020 Tipo de documento: Artigo País de afiliação: Estados Unidos