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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.

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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

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Date deposited: 19 Dec 2016 09:53
Last modified: 16 Mar 2024 03:51

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Contributors

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

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