Exact Exchange with Range-separated Algorithm for Thermodynamic Limit of Periodic Hartree-Fock Theory

Abstract

The expensive cost of computing exact exchange in periodic systems limits the application range of density functional theory with hybrid functionals. To reduce the computational cost of exact change, we present a range-separated algorithm to compute electron repulsion integrals for Gaussian-type crystal basis. The algorithm splits the full-range Coulomb interactions into short-range and long-range parts, which are respectively computed in real and reciprocal space. This approach significantly reduces the overall computational cost as integrals can be efficiently computed in both regions. The algorithm can efficiently handle large numbers of k points with limited CPU and memory resources. As a demonstration, we performed an all-electron k-point Hartree-Fock calculation for LiH crystal with 1 million Gaussian basis functions, which was completed on a desktop computer in 1400 CPU hours.

References in corpus (10)

• The Individual and Collective Effects of Exact Exchange and Dispersion Interactions on the Ab Initio Structure of Liquid Water
• Order-N implementation of exact exchange in extended systems
• Ideal regularization of the Coulomb singularity in exact exchange by Wigner-Seitz truncated interactions: towards chemical accuracy in non-trivial systems
• Gaussian and plane-wave mixed density fitting for periodic systems
• Projector augmented-wave and all-electron calculations across the periodic table: a comparison of structural and energetic properties
• Fast periodic Gaussian density fitting by range separation
• Relativistic Self-Consistent $GW$: Exact Two-Component Formalism with One-Electron Approximation for Solids
• Integral-direct Hartree-Fock and Møller-Plesset Perturbation Theory for Periodic Systems with Density Fitting: Application to the Benzene Crystal
• Various integral estimations and screening schemes for extended systems in PySCF
• Tight distance-dependent estimators for screening two-center and three-center short-range Coulomb integrals over Gaussian basis functions