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dc.contributor.authorKadek, Marius
dc.contributor.authorRepisky, Michal
dc.contributor.authorRuud, Kenneth
dc.date.accessioned2019-08-07T07:47:02Z
dc.date.available2019-08-07T07:47:02Z
dc.date.issued2019-05-03
dc.description.abstractWe present the first full-potential method that solves the fully relativistic four-component Dirac-Kohn-Sham equation for materials in the solid state within the framework of atom-centered Gaussian-type orbitals (GTOs). Our GTO-based method treats one-, two-, and three-dimensional periodic systems on an equal footing, and allows for a seamless transition to the methodology commonly used in studies of molecules with heavy elements. The scalar relativistic effects as well as the spin-orbit interaction are handled variationally. The full description of the electron-nuclear potential in the core region of heavy nuclei is straightforward due to the local nature of the GTOs and does not pose any computational difficulties. We show how the time-reversal symmetry and a quaternion algebra-based formalism can be exploited to significantly reduce the increased methodological complexity and computational cost associated with multiple wave-function components coupled by the spin-orbit interaction. We provide a detailed description of how to employ the matrix form of the multipole expansion and an iterative renormalization procedure to evaluate the conditionally convergent infinite lattice sums arising in studies of periodic systems. Next, we investigate the problem of inverse variational collapse that arises if the Dirac operator containing a repulsive periodic potential is expressed in a basis that includes diffuse functions, and suggest a possible solution. Finally, we demonstrate the validity of the method on three-dimensional silver halide (AgX) crystals with large relativistic effects and two-dimensional honeycomb structures (silicene and germanene) exhibiting the spin-orbit-driven quantum spin Hall effect. Our results are well-converged with respect to the basis set limit using standard bases developed for molecular calculations and indicate that the common rule of removing basis functions with small exponents should not be applied when transferring the molecular basis to solids.en_US
dc.description.sponsorshipTromsø Research Foundation Norwegian Supercomputer Program NOTUR Ministry of Education, Youth and Sports of the Czech Republic Publication fund of UiT The Arctic University of Norwayen_US
dc.descriptionSource at <a href=https://doi.org/10.1103/PhysRevB.99.205103>https://doi.org/10.1103/PhysRevB.99.205103</a>.en_US
dc.identifier.citationKadek, M., Repisky, M. & Ruud, K. (2019). All-electron fully relativistic Kohn-Sham theory for solids based on the Dirac-Coulomb Hamiltonian and Gaussian-type functions. <i>Physical Review B, 99</i>, 205103. https://doi.org/10.1103/PhysRevB.99.205103en_US
dc.identifier.cristinIDFRIDAID 1697892
dc.identifier.issn2469-9950
dc.identifier.issn2469-9969
dc.identifier.urihttps://hdl.handle.net/10037/15861
dc.language.isoengen_US
dc.publisherAmerican Physical Societyen_US
dc.relation.journalPhysical Review B
dc.relation.projectIDinfo:eu-repo/grantAgreement/RCN/SFF/179568/Norway/Centre for Theoretical and Computational Chemistry/CTCC/en_US
dc.relation.projectIDinfo:eu-repo/grantAgreement/RCN/SFF/262695/Norway/Hylleraas Centre for Quantum Molecular Sciences//en_US
dc.relation.projectIDinfo:eu-repo/grantAgreement/RCN/FRINATEK/214095/Norway/Relativistic two- and four-component density functional theory with periodic boundary conditions//en_US
dc.rights.accessRightsopenAccessen_US
dc.subjectVDP::Mathematics and natural science: 400::Chemistry: 440::Theoretical chemistry, quantum chemistry: 444en_US
dc.subjectVDP::Matematikk og Naturvitenskap: 400::Kjemi: 440::Teoretisk kjemi, kvantekjemi: 444en_US
dc.titleAll-electron fully relativistic Kohn-Sham theory for solids based on the Dirac-Coulomb Hamiltonian and Gaussian-type functionsen_US
dc.typeJournal articleen_US
dc.typeTidsskriftartikkelen_US
dc.typePeer revieweden_US


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