The University of Southampton
University of Southampton Institutional Repository

Perspective: Methods for large-scale density functional calculations on metallic systems

Perspective: Methods for large-scale density functional calculations on metallic systems
Perspective: Methods for large-scale density functional calculations on metallic systems
Current research challenges in areas such as energy and bioscience have created a strong need for Density Functional Theory (DFT) calculations on metallic nanostructures of hundreds to thousands of atoms to provide understanding at the atomic level in technologically important processes such as catalysis and magnetic materials. Linear-scaling DFT methods for calculations with thousands of atoms on insulators are now reaching a level of maturity. However such methods are not applicable to metals, where the continuum of states through the chemical potential and their partial occupancies provide significant hurdles which have yet to be fully overcome. Within this perspective we outline the theory of DFT calculations on metallic systems with a focus on methods for large-scale
calculations, as required for the study of metallic nanoparticles. We present early approaches for electronic energy minimization in metallic systems as well as approaches which can impose partial state occupancies from a thermal distribution without access to the electronic Hamiltonian eigenvalues, such as the classes of Fermi Operator Expansions and Integral Expansions. We then focus on the significant progress which has been made in the last decade with developments which promise to better tackle the length-scale problem in metals. We discuss the challenges presented by each method, the likely future directions that could be followed and whether an accurate linear-scaling
DFT method for metals is in sight.
0021-9606
1-14
Aarons, Jolyon
93e68133-73b0-43e0-8c91-464920f4a503
Sarwar, Misbah
ae93ef8f-8a84-4a46-95ac-cd9352c44e56
Thompsett, David
2fba717f-67ed-4999-b400-3c3a0681778f
Skylaris, Chris
8f593d13-3ace-4558-ba08-04e48211af61
Aarons, Jolyon
93e68133-73b0-43e0-8c91-464920f4a503
Sarwar, Misbah
ae93ef8f-8a84-4a46-95ac-cd9352c44e56
Thompsett, David
2fba717f-67ed-4999-b400-3c3a0681778f
Skylaris, Chris
8f593d13-3ace-4558-ba08-04e48211af61

Aarons, Jolyon, Sarwar, Misbah, Thompsett, David and Skylaris, Chris (2016) Perspective: Methods for large-scale density functional calculations on metallic systems. The Journal of Chemical Physics, 145 (22), 1-14. (doi:10.1063/1.4972007).

Record type: Article

Abstract

Current research challenges in areas such as energy and bioscience have created a strong need for Density Functional Theory (DFT) calculations on metallic nanostructures of hundreds to thousands of atoms to provide understanding at the atomic level in technologically important processes such as catalysis and magnetic materials. Linear-scaling DFT methods for calculations with thousands of atoms on insulators are now reaching a level of maturity. However such methods are not applicable to metals, where the continuum of states through the chemical potential and their partial occupancies provide significant hurdles which have yet to be fully overcome. Within this perspective we outline the theory of DFT calculations on metallic systems with a focus on methods for large-scale
calculations, as required for the study of metallic nanoparticles. We present early approaches for electronic energy minimization in metallic systems as well as approaches which can impose partial state occupancies from a thermal distribution without access to the electronic Hamiltonian eigenvalues, such as the classes of Fermi Operator Expansions and Integral Expansions. We then focus on the significant progress which has been made in the last decade with developments which promise to better tackle the length-scale problem in metals. We discuss the challenges presented by each method, the likely future directions that could be followed and whether an accurate linear-scaling
DFT method for metals is in sight.

Text
pdf_archiveJCPSA6vol_145iss_22220901_1_am.pdf - Accepted Manuscript
Download (3MB)

More information

Accepted/In Press date: 28 November 2016
e-pub ahead of print date: 15 December 2016
Organisations: Faculty of Natural and Environmental Sciences

Identifiers

Local EPrints ID: 403965
URI: http://eprints.soton.ac.uk/id/eprint/403965
ISSN: 0021-9606
PURE UUID: ac052bef-14e0-4409-9f01-157b85458d9d
ORCID for Chris Skylaris: ORCID iD orcid.org/0000-0003-0258-3433

Catalogue record

Date deposited: 19 Dec 2016 09:53
Last modified: 17 Jul 2018 00:32

Export record

Altmetrics

Contributors

Author: Jolyon Aarons
Author: Misbah Sarwar
Author: David Thompsett
Author: Chris Skylaris ORCID iD

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.

×