2025/07/13 by Andrew X. Zhu, Zhu, Andrew, Arman Nejad +7
Computer Science · #Chemical Physics (physics.chem-ph) #Computational Physics (physics.comp-ph) #FOS: Physical sciences #Materials Science (cond-mat.mtrl-sci) #Matrix Theory and Algorithms #Neural Networks and Applications
paper · pdf · doi:10.48550/arxiv.2507.09814
openalex publication_date 2025/07/13 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
We present a domain-based local pair natural orbital Møller--Plesset second order perturbation theory (DLPNO-MP2) for periodic systems, working within an LCAO formalism within the Tubromole program package. This approach, Megacell-DLPNO-MP2, embeds a supercell correlation treatment within a megacell and does not involve periodic image summation for the Coulomb integrals. Working in a basis of well-localised Wannier functions, periodicity is instead imposed through rigorous translational symmetry of Hamiltonian integrals and wavefunction parameters. The accuracy of the method is validated through comparison with a complementary periodic DLPNO-MP2 method that employs Born--von Kármán boundary conditions, described in paper I of this series. The PNO approximations are shown to be equivalent in the two approaches and entirely consistent with molecular DLPNO-MP2 calculations. The Megacell-DLPNO-MP2 method displays sub-linear scaling with respect to supercell size at the asymptotic limit and example calculations are presented with up to 15000 basis functions in the correlation treatment.