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

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

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
Publication status	Published - 2019

Bibliographical note

Funding Information:
† 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).

Funding Information:
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).

Publisher Copyright:
© 2019 the Owner Societies.

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

Access to Document

10.1039/c8cp03581d

Cite this

@article{33e5c93782804015a8d1d8d09598c7a3,

title = "Magnetic structure of UO2 and NpO2 by first-principle methods",

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.",

author = "Pegg, {James T.} and Shields, {Ashley E.} and Storr, {Mark T.} and Wills, {Andrew S.} and Scanlon, {David O.} and {De Leeuw}, {Nora H.}",

note = "Funding Information: † 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). Funding Information: 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{\textquoteright}s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202). Publisher Copyright: {\textcopyright} 2019 the Owner Societies.",

year = "2019",

doi = "10.1039/c8cp03581d",

language = "English",

volume = "21",

pages = "760--771",

journal = "Physical Chemistry Chemical Physics",

issn = "1463-9076",

publisher = "Royal Society of Chemistry",

number = "2",

}

TY - JOUR

T1 - Magnetic structure of UO2 and NpO2 by first-principle methods

AU - Pegg, James T.

AU - Shields, Ashley E.

AU - Storr, Mark T.

AU - Wills, Andrew S.

AU - Scanlon, David O.

AU - De Leeuw, Nora H.

N1 - Funding Information: † 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). Funding Information: 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). Publisher Copyright: © 2019 the Owner Societies.

PY - 2019

Y1 - 2019

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85059421560&partnerID=8YFLogxK

U2 - 10.1039/c8cp03581d

DO - 10.1039/c8cp03581d

M3 - Article

C2 - 30547167

AN - SCOPUS:85059421560

SN - 1463-9076

VL - 21

SP - 760

EP - 771

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

IS - 2

ER -