+ Site Statistics
+ Search Articles
+ PDF Full Text Service
How our service works
Request PDF Full Text
+ Follow Us
Follow on Facebook
Follow on Twitter
Follow on LinkedIn
+ Subscribe to Site Feeds
Most Shared
PDF Full Text
+ Translate
+ Recently Requested

Local Fitting of the Kohn-Sham Density in a Gaussian and Plane Waves Scheme for Large-Scale Density Functional Theory Simulations

Local Fitting of the Kohn-Sham Density in a Gaussian and Plane Waves Scheme for Large-Scale Density Functional Theory Simulations

Journal of Chemical Theory and Computation 13(5): 2202-2214

A local resolution-of-the-identity (LRI) approach is introduced in combination with the Gaussian and plane waves (GPW) scheme to enable large-scale Kohn-Sham density functional theory calculations. In GPW, the computational bottleneck is typically the description of the total charge density on real-space grids. Introducing the LRI approximation, the linear scaling of the GPW approach with respect to system size is retained, while the prefactor for the grid operations is reduced. The density fitting is an O(N) scaling process implemented by approximating the atomic pair densities by an expansion in one-center fit functions. The computational cost for the grid-based operations becomes negligible in LRIGPW. The self-consistent field iteration is up to 30 times faster for periodic systems dependent on the symmetry of the simulation cell and on the density of grid points. However, due to the overhead introduced by the local density fitting, single point calculations and complete molecular dynamics steps, including the calculation of the forces, are effectively accelerated by up to a factor of ∼10. The accuracy of LRIGPW is assessed for different systems and properties, showing that total energies, reaction energies, intramolecular and intermolecular structure parameters are well reproduced. LRIGPW yields also high quality results for extended condensed phase systems such as liquid water, ice XV, and molecular crystals.

Please choose payment method:

(PDF emailed within 0-6 h: $19.90)

Accession: 059923183

Download citation: RISBibTeXText

PMID: 28383917

DOI: 10.1021/acs.jctc.7b00148

Related references

Hybrid ab initio Kohn-Sham density functional theory/frozen-density orbital-free density functional theory simulation method suitable for biological systems. Journal of Chemical Physics 128(1): 014101, 2008

Tight-binding density functional theory: an approximate Kohn-Sham DFT scheme. Journal of Physical Chemistry. a 111(26): 5609-5613, 2007

Restoration of the derivative discontinuity in Kohn-Sham density functional theory: an efficient scheme for energy gap correction. Physical Review Letters 110(3): 033002, 2013

MN15-L: A New Local Exchange-Correlation Functional for Kohn-Sham Density Functional Theory with Broad Accuracy for Atoms, Molecules, and Solids. Journal of Chemical Theory and Computation 12(3): 1280-1293, 2016

Increasing the applicability of density functional theory. III. Do consistent Kohn-Sham density functional methods exist?. Journal of Chemical Physics 137(13): 134102, 2012

Multiconfiguration Pair-Density Functional Theory Outperforms Kohn-Sham Density Functional Theory and Multireference Perturbation Theory for Ground-State and Excited-State Charge Transfer. Journal of Chemical Theory and Computation 11(8): 3643-3649, 2015

Mechanism of Oxygenase-Pathway Reactions Catalyzed by Rubisco from Large-Scale Kohn-Sham Density Functional Calculations. Journal of Physical Chemistry. B 123(13): 2833-2843, 2019

Adaptive local basis set for Kohn-Sham density functional theory in a discontinuous Galerkin framework I Total energy calculation. Journal of Computational Physics 231(4): 2140-2154, 2012

Poisson-transformed density fitting in relativistic four-component Dirac-Kohn-Sham theory. Journal of Chemical Physics 128(12): 124108, 2008

Self-interaction correction in a real-time Kohn-Sham scheme: access to difficult excitations in time-dependent density functional theory. Journal of Chemical Physics 137(6): 064117, 2012

A density matrix-based quasienergy formulation of the Kohn-Sham density functional response theory using perturbation- and time-dependent basis sets. Journal of Chemical Physics 129(21): 214108, 2008

Density-Fitting Method in Symmetry-Adapted Perturbation Theory Based on Kohn-Sham Description of Monomers. Journal of Chemical Theory and Computation 2(2): 400-412, 2006

A density matrix-based method for the linear-scaling calculation of dynamic second- and third-order properties at the Hartree-Fock and Kohn-Sham density functional theory levels. Journal of Chemical Physics 127(20): 204103, 2007

Plane-wave pseudopotential implementation of explicit integrators for time-dependent Kohn-Sham equations in large-scale simulations. Journal of Chemical Physics 137(22): 22a546, 2012

On the diagnostic value of ( 2 ) in Kohn-Sham density functional theory. Molecular Physics 99(11): 981-989, 2001