title: A third-generation density-functional-theory-based method for calculating canonical molecular orbitals of large molecules.
abstract: We used grid-free modified Cholesky decomposition (CD) to develop a density-functional-theory (DFT)-based method for calculating the canonical molecular orbitals (CMOs) of large molecules. Our method can be used to calculate standard CMOs, analytically compute exchange-correlation terms, and maximise the capacity of next-generation supercomputers. Cholesky vectors were first analytically downscaled using low-rank pivoted CD and CD with adaptive metric (CDAM). The obtained Cholesky vectors were distributed and stored on each computer node in a parallel computer, and the Coulomb, Fock exchange, and pure exchange-correlation terms were calculated by multiplying the Cholesky vectors without evaluating molecular integrals in self-consistent field iterations. Our method enables DFT and massively distributed memory parallel computers to be used in order to very efficiently calculate the CMOs of large molecules.
authors.affiliation: Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro, Tokyo 153-8505, Japan. satofumi@iis.u-tokyo.ac.jp.
authors.forename: Toshiyuki
authors.initials: T
authors.lastname: Hirano
authors.forename: Fumitoshi
authors.initials: F
authors.lastname: Sato
mesh_terms: D000409:Alanine / Q000737:chemistry*; D009842:Oligopeptides / Q000737:chemistry*; D011789:Quantum Theory
chemical_list: D009842:Oligopeptides; C047981:arginyl-glycyl-aspartic acid; D000409:Alanine