Efficient distance-including integral screening in linear-scaling Møller-Plesset perturbation theory

Area of Science:

• Computational Chemistry
• Quantum Chemistry
• Theoretical Chemistry

Background:

• Møller-Plesset perturbation theory (MP2) is crucial for accurate electronic structure calculations.
• Conventional MP2 methods exhibit high computational cost, scaling poorly with system size.
• Efficient preselection of two-electron integrals is key to reducing computational burden.

Purpose of the Study:

• To develop efficient integral estimates for atomic-orbital based Møller-Plesset perturbation theory (AO-MP2).
• To achieve linear scaling computational effort for AO-MP2 energy calculations.
• To enable accurate calculations on large molecular systems.

Main Methods:

• Utilizing the QQR approach for integral preselection.
• Exploiting asymptotic decay of integral values with bra-ket separation.
• Combining multipole expansion insights with Schwarz bounds for tight estimates.

Main Results:

• Demonstrated reliable AO-MP2 energy calculations for systems with localized and delocalized electronic structures.
• Achieved early onset of linear scaling for systems with localized electronic structure, such as DNA.
• Enabled computation of systems with over 1000 atoms and 10,000 basis functions on a single core.

Conclusions:

• The developed AO-MP2 method with QQR-type estimates offers significant computational advantages.
• This approach makes large-scale electronic structure calculations feasible and accurate.
• The method is well-suited for parallelization, demonstrated on a large protein-DNA complex.