Header

UZH-Logo

Maintenance Infos

Efficient periodic resolution-of-the-identity Hartree–Fock exchange method with k-point sampling and Gaussian basis sets


Bussy, Augustin; Hutter, Jürg (2024). Efficient periodic resolution-of-the-identity Hartree–Fock exchange method with k-point sampling and Gaussian basis sets. Journal of Chemical Physics, 160(6):064116.

Abstract

Simulations of condensed matter systems at the hybrid density functional theory level pose significant computational challenges. The elevated costs arise from the non-local nature of the Hartree–Fock exchange (HFX) in conjunction with the necessity to approach the thermodynamic limit. In this work, we address these issues with the development of a new efficient method for the calculation of HFX in periodic systems, employing k-point sampling. We rely on a local atom-specific resolution-of-the-identity scheme, the use of atom-centered Gaussian type orbitals, and the truncation of the Coulomb interaction to limit computational complexity. Our real-space approach exhibits a scaling that is, at worst, linear with the number of k-points. Issues related to basis set diffuseness are effectively addressed through the auxiliary density matrix method. We report the implementation in the CP2K software package, as well as accuracy and performance benchmarks. This method demonstrates excellent agreement with equivalent Γ-point supercell calculations in terms of relative energies and nuclear gradients. Good strong and weak scaling performances, as well as graphics processing unit (GPU) acceleration, make this implementation a promising candidate for high-performance computing.

Abstract

Simulations of condensed matter systems at the hybrid density functional theory level pose significant computational challenges. The elevated costs arise from the non-local nature of the Hartree–Fock exchange (HFX) in conjunction with the necessity to approach the thermodynamic limit. In this work, we address these issues with the development of a new efficient method for the calculation of HFX in periodic systems, employing k-point sampling. We rely on a local atom-specific resolution-of-the-identity scheme, the use of atom-centered Gaussian type orbitals, and the truncation of the Coulomb interaction to limit computational complexity. Our real-space approach exhibits a scaling that is, at worst, linear with the number of k-points. Issues related to basis set diffuseness are effectively addressed through the auxiliary density matrix method. We report the implementation in the CP2K software package, as well as accuracy and performance benchmarks. This method demonstrates excellent agreement with equivalent Γ-point supercell calculations in terms of relative energies and nuclear gradients. Good strong and weak scaling performances, as well as graphics processing unit (GPU) acceleration, make this implementation a promising candidate for high-performance computing.

Statistics

Citations

Altmetrics

Downloads

4 downloads since deposited on 01 Mar 2024
5 downloads since 12 months
Detailed statistics

Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > General Physics and Astronomy
Physical Sciences > Physical and Theoretical Chemistry
Uncontrolled Keywords:Physical and Theoretical Chemistry, General Physics and Astronomy
Language:English
Date:14 February 2024
Deposited On:01 Mar 2024 13:15
Last Modified:30 Jun 2024 03:38
Publisher:American Institute of Physics
ISSN:0021-9606
OA Status:Hybrid
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1063/5.0189659
PubMed ID:38353305
Project Information:
  • : FunderSwiss Platform for Advanced Scientific Computing
  • : Grant ID
  • : Project Title
  • Content: Published Version
  • Language: English
  • Licence: Creative Commons: Attribution 4.0 International (CC BY 4.0)