Extension and acceleration of relativistic density functional theory based on transformed density operator

Yasuhiro Ikabata, Takuro Oyama, Masao Hayami, Junji Seino, Hiromi Nakai

Research output: Contribution to journalArticle

Abstract

We report an extension of relativistic density functional theory (RDFT) within one-component or two-component expressions that relies on a unitary-transformed density operator as well as a unitary-transformed Hamiltonian [Oyama et al., Chem. Phys. Lett. 680, 37 (2017)]. The transformed density operator is introduced to avoid the picture-change effect in the electron density, density gradient, kinetic energy density, and exchange-correlation potential. We confirmed that the implementation based on the spin-free infinite-order Douglas-Kroll-Hess method gives total, orbital, and excitation energies close to the reference values given by four-component RDFT calculations. To reduce the computational cost due to the transformed density operator, the local unitary transformation was also implemented. Numerical assessments revealed that the present scheme enabled the RDFT calculation of polyatomic systems with negligibly small picture-change effect.

Original languageEnglish
Article number164104
JournalJournal of Chemical Physics
Volume150
Issue number16
DOIs
Publication statusPublished - 2019 Apr 28

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Density functional theory
Mathematical operators
density functional theory
operators
Hamiltonians
Excitation energy
Kinetic energy
Carrier concentration
flux density
kinetic energy
energy transfer
costs
orbitals
gradients
Costs
excitation
energy

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Extension and acceleration of relativistic density functional theory based on transformed density operator. / Ikabata, Yasuhiro; Oyama, Takuro; Hayami, Masao; Seino, Junji; Nakai, Hiromi.

In: Journal of Chemical Physics, Vol. 150, No. 16, 164104, 28.04.2019.

Research output: Contribution to journalArticle

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