title: Tensor Hypercontraction Second-Order Møller-Plesset Perturbation Theory: Grid Optimization and Reaction Energies.
abstract: We have recently introduced the tensor hypercontraction (THC) method for electronic structure, including MP2. Here, we present an algorithm for THC-MP2 that lowers the memory requirements as well as the prefactor while maintaining the formal quartic scaling that we demonstrated previously. We also describe a procedure to optimize quadrature grids used in grid-based least-squares (LS) THC-MP2. We apply this algorithm to generate grids for first-row atoms with less than 100 points/atom while incurring negligible errors in the computed energies. We benchmark the LS-THC-MP2 method using optimized grids for a wide variety of tests sets including conformational energies and reaction barriers in both the cc-pVDZ and cc-pVTZ basis sets. These tests demonstrate that the THC methodology is not limited to small basis sets and that it incurs negligible errors in both absolute and relative energies.
authors.affiliation: Department of Chemistry and the PULSE Institute, Stanford University , Stanford, California 94305, United States.|SLAC National Accelerator Laboratory , Menlo Park, California 94025, United States.
authors.forename: Sara I L Kokkila
authors.initials: SI
authors.lastname: Schumacher
authors.affiliation: Department of Chemistry and the PULSE Institute, Stanford University , Stanford, California 94305, United States.|SLAC National Accelerator Laboratory , Menlo Park, California 94025, United States.|Department of Chemistry and Biochemistry, City College of New York , New York, New York 10031, United States.
authors.forename: Edward G
authors.initials: EG
authors.lastname: Hohenstein
authors.affiliation: Center for Computational Molecular Science and Technology, School of Chemistry and Biochemistry, Georgia Institute of Technology , Atlanta, Georgia 30332-0400, United States.
authors.forename: Robert M
authors.initials: RM
authors.lastname: Parrish
authors.affiliation: Department of Chemistry and the PULSE Institute, Stanford University , Stanford, California 94305, United States.|SLAC National Accelerator Laboratory , Menlo Park, California 94025, United States.
authors.forename: Lee-Ping
authors.initials: LP
authors.lastname: Wang
authors.affiliation: Department of Chemistry and the PULSE Institute, Stanford University , Stanford, California 94305, United States.|SLAC National Accelerator Laboratory , Menlo Park, California 94025, United States.
authors.forename: Todd J
authors.initials: TJ
authors.lastname: Martínez