Linear-scaling implementation of the direct random-phase approximation

Research output: Contribution to journalArticle

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Abstract

We report the linear-scaling implementation of the direct random-phase approximation (dRPA) for closed-shell molecular systems. As a bonus, linear-scaling algorithms are also presented for the second-order screened exchange extension of dRPA as well as for the second-order Møller-Plesset (MP2) method and its spin-scaled variants. Our approach is based on an incremental scheme which is an extension of our previous local correlation method [Rolik et al., J. Chem. Phys. 139, 094105 (2013)]. The approach extensively uses local natural orbitals to reduce the size of the molecular orbital basis of local correlation domains. In addition, we also demonstrate that using natural auxiliary functions [M. Kállay, J. Chem. Phys. 141, 244113 (2014)], the size of the auxiliary basis of the domains and thus that of the three-center Coulomb integral lists can be reduced by an order of magnitude, which results in significant savings in computation time. The new approach is validated by extensive test calculations for energies and energy differences. Our benchmark calculations also demonstrate that the new method enables dRPA calculations for molecules with more than 1000 atoms and 10000 basis functions on a single processor.

Original languageEnglish
Article number204105
JournalThe Journal of Chemical Physics
Volume142
Issue number20
DOIs
Publication statusPublished - May 28 2015

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scaling
approximation
Correlation methods
Molecular orbitals
lists
central processing units
molecular orbitals
orbitals
Atoms
Molecules
energy
atoms
molecules

ASJC Scopus subject areas

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

Cite this

Linear-scaling implementation of the direct random-phase approximation. / Kállay, M.

In: The Journal of Chemical Physics, Vol. 142, No. 20, 204105, 28.05.2015.

Research output: Contribution to journalArticle

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