The University of Southampton
University of Southampton Institutional Repository

A variational method for density functional theory calculations on metallic systems with thousands of atoms

A variational method for density functional theory calculations on metallic systems with thousands of atoms
A variational method for density functional theory calculations on metallic systems with thousands of atoms
A new method for finite-temperature density functional theory calculations which significantly increases the number of atoms that can be simulated in metallic systems is presented. A self-consistent, direct minimization technique is used to obtain the Helmholtz free energy of the electronic system, described in terms of a set of non-orthogonal, localized functions which are optimized in situ using a periodic-sinc basis set, equivalent to plane waves. Most parts of the calculation, including the demanding operation of building the Hamiltonian matrix, have a computational cost that scales linearly with the number of atoms in the system. Also, this approach ensures that the Hamiltonian matrix has a minimal size, which reduces the computational overhead due to diagonalization, a cubic-scaling operation that is still required. Large basis set accuracy is retained via the optimization of the localized functions. This method allows accurate simulations of entire metallic nanostructures, demonstrated with calculations on a supercell of bulk copper with 500 atoms and on gold nanoparticles with up to 2057 atoms
0021-9606
54107
Ruiz-Serrano, A.
17faa8c3-e6a4-4d31-93e0-a86e7bd84830
Skylaris, C.-K.
8f593d13-3ace-4558-ba08-04e48211af61
Ruiz-Serrano, A.
17faa8c3-e6a4-4d31-93e0-a86e7bd84830
Skylaris, C.-K.
8f593d13-3ace-4558-ba08-04e48211af61

Ruiz-Serrano, A. and Skylaris, C.-K. (2013) A variational method for density functional theory calculations on metallic systems with thousands of atoms The Journal of Chemical Physics, 139, (5), p. 54107. (doi:10.1063/1.4817001).

Record type: Article

Abstract

A new method for finite-temperature density functional theory calculations which significantly increases the number of atoms that can be simulated in metallic systems is presented. A self-consistent, direct minimization technique is used to obtain the Helmholtz free energy of the electronic system, described in terms of a set of non-orthogonal, localized functions which are optimized in situ using a periodic-sinc basis set, equivalent to plane waves. Most parts of the calculation, including the demanding operation of building the Hamiltonian matrix, have a computational cost that scales linearly with the number of atoms in the system. Also, this approach ensures that the Hamiltonian matrix has a minimal size, which reduces the computational overhead due to diagonalization, a cubic-scaling operation that is still required. Large basis set accuracy is retained via the optimization of the localized functions. This method allows accurate simulations of entire metallic nanostructures, demonstrated with calculations on a supercell of bulk copper with 500 atoms and on gold nanoparticles with up to 2057 atoms

Other 1/jcpsa6/v139/i5/p054107_s1 - Version of Record
Download (243kB)

More information

Published date: 2013
Organisations: Computational Systems Chemistry

Identifiers

Local EPrints ID: 356350
URI: http://eprints.soton.ac.uk/id/eprint/356350
ISSN: 0021-9606
PURE UUID: ba87a2b4-629d-4473-bbbb-3afcb9f5e2f9

Catalogue record

Date deposited: 06 Sep 2013 08:40
Last modified: 18 Jul 2017 03:39

Export record

Altmetrics

Contributors

Author: A. Ruiz-Serrano
Author: C.-K. Skylaris

University divisions

Download statistics

Downloads from ePrints over the past year. Other digital versions may also be available to download e.g. from the publisher's website.

View more statistics

Atom RSS 1.0 RSS 2.0

Contact ePrints Soton: eprints@soton.ac.uk

ePrints Soton supports OAI 2.0 with a base URL of http://eprints.soton.ac.uk/cgi/oai2

This repository has been built using EPrints software, developed at the University of Southampton, but available to everyone to use.

We use cookies to ensure that we give you the best experience on our website. If you continue without changing your settings, we will assume that you are happy to receive cookies on the University of Southampton website.

×