Magnetic structure of UO2 and NpO2 by first-principle methods

James T. Pegg; Ashley E. Shields; Mark T. Storr; Andrew S. Wills; David O. Scanlon; Nora H. De Leeuw

doi:10.1039/c8cp03581d

Magnetic structure of UO₂ and NpO₂ by first-principle methods

James T. Pegg, Ashley E. Shields, Mark T. Storr, Andrew S. Wills, David O. Scanlon, Nora H. De Leeuw

Materials & Chemistry Group

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32 Scopus citations

Abstract

The magnetic structure of the actinide dioxides (AnO₂) remains a field of intense research. A low-temperature experimental investigation of the magnetic ground-state is complicated by thermal energy released from the radioactive decay of the actinide nuclei. To establish the magnetic ground-state, we have employed high-accuracy computational methods to systematically probe different magnetic structures. A transverse 1k antiferromagnetic ground-state with Fmmm (No. 69) crystal symmetry has been established for UO₂, whereas a ferromagnetic (111) ground-state with R3m (No. 166) has been established for NpO₂. Band structure calculations have been performed to analyse these results.

Original language	English
Pages (from-to)	760-771
Number of pages	12
Journal	Physical Chemistry Chemical Physics
Volume	21
Issue number	2
DOIs	https://doi.org/10.1039/c8cp03581d
State	Published - 2019

Funding

† Electronic supplementary information (ESI) available. See DOI: 10.1039/c8cp03581d ‡ This manuscript has been co-authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This research was supported by the UK Engineering & Physical Science Research Council (EPSRC) (Grant no. EP/G036675 and EP/K016288) and the Atomic Weapons Establishment (AWE). AES gratefully acknowledges the United States Department of Homeland Security (DHS), Domestic Nuclear Detection Office (DNDO), National Technical Nuclear Forensics Centre (NTNFC), for a Postdoctoral Research Fellowship. NHdL thanks AWE for a William Penney Fellowship. This work made use of the ARCHER UK National Supercomputing Service (http://www.archer.ac.uk), via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202).

Funders	Funder number
Domestic Nuclear Detection Office
Engineering & Physical Science Research Council
National Technical Nuclear Forensics Centre
US Department of Energy
U.S. Department of Energy
U.S. Department of Homeland Security
Design History Society
Atomic Weapons Establishment	EP/L000202

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abstract = "The magnetic structure of the actinide dioxides (AnO2) remains a field of intense research. A low-temperature experimental investigation of the magnetic ground-state is complicated by thermal energy released from the radioactive decay of the actinide nuclei. To establish the magnetic ground-state, we have employed high-accuracy computational methods to systematically probe different magnetic structures. A transverse 1k antiferromagnetic ground-state with Fmmm (No. 69) crystal symmetry has been established for UO2, whereas a ferromagnetic (111) ground-state with R3m (No. 166) has been established for NpO2. Band structure calculations have been performed to analyse these results.",

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AU - Shields, Ashley E.

AU - Storr, Mark T.

AU - Wills, Andrew S.

AU - Scanlon, David O.

AU - De Leeuw, Nora H.

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ER -

Magnetic structure of UO₂ and NpO₂ by first-principle methods

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