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dc.contributor.authorZang, Xiaoning
dc.contributor.authorSchwingenschlögl, Udo
dc.contributor.authorLusk, Mark T.
dc.date.accessioned2020-02-06T11:52:05Z
dc.date.available2020-02-06T11:52:05Z
dc.date.issued2020-01-15
dc.date.submitted2019-05-01
dc.identifier.citationZang, X., Schwingenschlögl, U., & Lusk, M. T. (2020). Identification and Resolution of Unphysical Multielectron Excitations in the Real-Time Time-Dependent Kohn-Sham Formulation. Physical Review Letters, 124(2). doi:10.1103/physrevlett.124.026402
dc.identifier.doi10.1103/PhysRevLett.124.026402
dc.identifier.urihttp://hdl.handle.net/10754/661416
dc.description.abstractWe resolve a fundamental issue associated with the conventional Kohn-Sham formulation of real-time time-dependent density functional theory. We show that unphysical multielectron excitations, generated during time propagation of the Kohn-Sham equations due to fixation of the total number of Kohn-Sham orbitals and their occupations, result in incorrect electron density and, therefore, wrong predictions of physical properties. A new formulation is proposed in that the number of Kohn-Sham orbitals and their occupations are updated on the fly, the unphysical multielectron excitations are removed, and the correct electron density is determined. The correctness of the new formulation is demonstrated by simulations of Rabi oscillation, as analytical results are available for comparison in the case of noninteracting electrons.
dc.publisherAmerican Physical Society (APS)
dc.relation.urlhttps://link.aps.org/doi/10.1103/PhysRevLett.124.026402
dc.relation.urlhttp://arxiv.org/pdf/1912.10676
dc.rightsArchived with thanks to Physical Review Letters
dc.titleIdentification and Resolution of Unphysical Multielectron Excitations in the Real-Time Time-Dependent Kohn-Sham Formulation
dc.typeArticle
dc.contributor.departmentComputational Physics and Materials Science (CPMS)
dc.contributor.departmentMaterial Science and Engineering Program
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalPhysical Review Letters
dc.eprint.versionPublisher's Version/PDF
dc.contributor.institutionDepartment of Physics, Colorado School of Mines, Golden, Colorado 80401, USA
dc.identifier.arxivid1912.10676
kaust.personZang, Xiaoning
kaust.personSchwingenschlögl, Udo
refterms.dateFOA2020-02-06T11:52:44Z


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