Low-Scaling Tensor Hypercontraction in the Cholesky Molecular Orbital Basis Applied to Second-Order Moller-Plesset Perturbation Theory

Bangerter, Felix H.; Glasbrenner, Michael und Ochsenfeld, Christian (2021): Low-Scaling Tensor Hypercontraction in the Cholesky Molecular Orbital Basis Applied to Second-Order Moller-Plesset Perturbation Theory. In: Journal of Chemical Theory and Computation, Bd. 17, Nr. 1: S. 211-221

Abstract

We employ various reduced scaling techniques to accelerate the recently developed least-squares tensor hypercontraction (LS-THC) approximation [Parrish, R M., Hohenstein, E. G., Martinez, T. J., Sherrill, C. D. J. Chem. Phys. 137, 224106 (2012)] for electron repulsion integrals (ERIs) and apply it to second-order Moller-Plesset perturbation theory (MP2). The grid-projected ERI tensors are efficiently constructed using a localized Cholesky molecular orbital basis from density-fitted integrals with an attenuated Coulomb metric. Additionally, rigorous integral screening and the natural blocking matrix format are applied to reduce the complexity of this step. By recasting the equations to form the quantized representation of the 1/r operator Z into the form of a system of linear equations, the bottleneck of inverting the grid metric via pseudoinversion is removed. This leads to a reduced scaling THC algorithm and application to MP2 yields the (sub-)quadratically scaling THC-omega-RI-CDD-SOS-MP2 method. The efficiency of this method is assessed for various systems including DNA fragments with over 8000 basis functions and the subquadratic scaling is illustrated.

• Dokumententyp: Zeitschriftenartikel
• Fakultät: Chemie und Pharmazie > Department Chemie
• Themengebiete: 500 Naturwissenschaften und Mathematik > 540 Chemie
• ISSN: 1549-9618
• Sprache: Englisch