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Title: Hidden magnetic order in plutonium dioxide nuclear fuel


The magnetic structure of PuO2 has been investigated by computational methods. A hereto unknown longitudinal 3k AFM ground-state that retains $$Fm\bar{3}m$$ crystal symmetry has been identified.

ORCiD logo [1]; ORCiD logo [2];  [3];  [4]; ORCiD logo [5]; ORCiD logo [6]
  1. Univ. College London, London (United Kingdom); Atomic Weapons Establishment (AWE) Plc, Aldermaston (United Kingdom)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Atomic Weapons Establishment (AWE) Plc, Aldermaston (United Kingdom)
  4. Univ. College London, London (United Kingdom)
  5. Univ. College London, London (United Kingdom); Diamond Light Source Ltd., Didcot (United Kingdom)
  6. Univ. College London, London (United Kingdom); Cardiff Univ., Cardiff (United Kingdom)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
Grant/Contract Number:  
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 20; Journal Issue: 32; Journal ID: ISSN 1463-9076
Royal Society of Chemistry
Country of Publication:
United States

Citation Formats

Pegg, James T., Shields, Ashley E., Storr, Mark T., Wills, Andrew S., Scanlon, David O., and de Leeuw, Nora H. Hidden magnetic order in plutonium dioxide nuclear fuel. United States: N. p., 2018. Web. doi:10.1039/C8CP03583K.
Pegg, James T., Shields, Ashley E., Storr, Mark T., Wills, Andrew S., Scanlon, David O., & de Leeuw, Nora H. Hidden magnetic order in plutonium dioxide nuclear fuel. United States.
Pegg, James T., Shields, Ashley E., Storr, Mark T., Wills, Andrew S., Scanlon, David O., and de Leeuw, Nora H. Thu . "Hidden magnetic order in plutonium dioxide nuclear fuel". United States.
title = {Hidden magnetic order in plutonium dioxide nuclear fuel},
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.},
abstractNote = {The magnetic structure of PuO2 has been investigated by computational methods. A hereto unknown longitudinal 3k AFM ground-state that retains $Fm\bar{3}m$ crystal symmetry has been identified.},
doi = {10.1039/C8CP03583K},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 32,
volume = 20,
place = {United States},
year = {2018},
month = {7}

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Works referenced in this record:

Density functional theory calculations on magnetic properties of actinide compounds
journal, January 2010

  • Gryaznov, Denis; Heifets, Eugene; Sedmidubsky, David
  • Physical Chemistry Chemical Physics, Vol. 12, Issue 38
  • DOI: 10.1039/c0cp00372g

Crystal-field transition in PuO 2
journal, January 1999

Magnetic susceptibility and spin-lattice interactions in U 1 x Pu x O 2 single crystals
journal, December 2002

Hybrid functionals based on a screened Coulomb potential
journal, May 2003

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 118, Issue 18
  • DOI: 10.1063/1.1564060

Cooperativity among defect sites in A O 2 + x and A 4 O 9 ( A = U , Np , Pu ) : Density functional calculations
journal, January 2009

Helium behavior in oxide nuclear fuels: First principles modeling
journal, October 2010

  • Gryaznov, D.; Rashkeev, S.; Kotomin, E. A.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 268, Issue 19
  • DOI: 10.1016/j.nimb.2010.05.054

Self-radiation effects on the lattice parameter of 238PuO2
journal, January 1974

Antiferromagnetism. Theory of Superexchange Interaction
journal, July 1950

Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Lattice defects and magnetic ordering in plutonium oxides: A hybrid density-functional-theory study of strongly correlated materials
journal, July 2005

  • Prodan, Ionut D.; Scuseria, Gustavo E.; Sordo, José A.
  • The Journal of Chemical Physics, Vol. 123, Issue 1
  • DOI: 10.1063/1.1953427

Nonmagnetic ground state of PuO 2
journal, January 2014

Reaction of Plutonium Dioxide with Water: Formation and Properties of PuO2+x
journal, January 2000

Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators
journal, August 1995

Magnetic-Octupole Order in Neptunium Dioxide?
journal, September 2000

Electronic and mechanical properties of ordered (Pu, U) O2 compounds: A density functional theory +U study
journal, February 2013

Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)]
journal, June 2006

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 124, Issue 21
  • DOI: 10.1063/1.2204597

NMR studies of actinide dioxides
journal, October 2007

Puzzling Lack of Temperature Dependence of the PuO 2 Magnetic Susceptibility Explained According to Ab Initio Wave Function Calculations
journal, January 2017

Magnetic Susceptibilities of Uranium (IV) and Plutonium (IV) Ions in Cubic Fields
journal, January 1959

  • Candela, George A.; Hutchison, Clyde A.; Lewis, W. Burton
  • The Journal of Chemical Physics, Vol. 30, Issue 1
  • DOI: 10.1063/1.1729881

Unusual magnetism of NpO 2 : A study with resonant x-ray scattering
journal, December 1999

Susceptibilite magnetique de PuO2
journal, June 1968

Size effects on the electronic and magnetic properties of PuO 2 (111) surface
journal, January 2016

LDA+U study of Pu and PuO2 on ground state with spin–orbital coupling
journal, August 2012

Assessing the performance of recent density functionals for bulk solids
journal, April 2009

Fully relativistic density functional calculations on hydroxylated actinide oxide surfaces
journal, January 2002

  • Boettger, J. C.; Ray, A. K.
  • International Journal of Quantum Chemistry, Vol. 90, Issue 4-5
  • DOI: 10.1002/qua.10350

Optical band gap of NpO 2 and PuO 2 from optical absorbance of epitaxial films
journal, January 2013

  • Mark McCleskey, T.; Bauer, Eve; Jia, Quanxi
  • Journal of Applied Physics, Vol. 113, Issue 1
  • DOI: 10.1063/1.4772595

J dependence in the LSDA + U treatment of noncollinear magnets
journal, December 2010

Covalency in the actinide dioxides: Systematic study of the electronic properties using screened hybrid density functional theory
journal, July 2007

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965

A Screened Hybrid DFT Study of Actinide Oxides, Nitrides, and Carbides
journal, June 2013

  • Wen, Xiao-Dong; Martin, Richard L.; Scuseria, Gustavo E.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 25
  • DOI: 10.1021/jp403141t

journal, March 1955

  • Asprey, L. B.; Ellinger, F. H.; Fried, S.
  • Journal of the American Chemical Society, Vol. 77, Issue 6
  • DOI: 10.1021/ja01611a108

Electronic correlation and transport properties of nuclear fuel materials
journal, November 2011

Assessment of metageneralized gradient approximation and screened Coulomb hybrid density functionals on bulk actinide oxides
journal, January 2006

Influence of the exchange screening parameter on the performance of screened hybrid functionals
journal, December 2006

  • Krukau, Aliaksandr V.; Vydrov, Oleg A.; Izmaylov, Artur F.
  • The Journal of Chemical Physics, Vol. 125, Issue 22
  • DOI: 10.1063/1.2404663

Forces in Molecules
journal, August 1939

Special points for Brillouin-zone integrations
journal, June 1976

  • Monkhorst, Hendrik J.; Pack, James D.
  • Physical Review B, Vol. 13, Issue 12, p. 5188-5192
  • DOI: 10.1103/PhysRevB.13.5188

Crystal-field levels and magnetic susceptibility in PuO 2
journal, April 2002

Ground-state properties and high-pressure behavior of plutonium dioxide: Density functional theory calculations
journal, October 2010

Toward reliable density functional methods without adjustable parameters: The PBE0 model
journal, April 1999

  • Adamo, Carlo; Barone, Vincenzo
  • The Journal of Chemical Physics, Vol. 110, Issue 13
  • DOI: 10.1063/1.478522

Magnetic order in NpO2 and UO2 studied by muon spin rotation
journal, June 1998

Inhomogeneous Electron Gas
journal, November 1964

Band theory and Mott insulators: Hubbard U instead of Stoner I
journal, July 1991

  • Anisimov, Vladimir I.; Zaanen, Jan; Andersen, Ole K.
  • Physical Review B, Vol. 44, Issue 3, p. 943-954
  • DOI: 10.1103/PhysRevB.44.943

Neutron-Diffraction Study of U O 2 : Observation of an Internal Distortion
journal, December 1975

NMR Evidence for Triple- q Multipole Structure in NpO 2
journal, April 2005

DFT+U study of the structures and properties of the actinide dioxides
journal, August 2017

Magnetism of actinide compounds
journal, September 1999

Observation of 239Pu Nuclear Magnetic Resonance
journal, May 2012

Neutron diffraction study of U O 2 : Antiferromagnetic state
journal, August 1976

Thermodynamic stability of PuO 2 surfaces: Influence of electronic correlations
journal, November 2011

Dynamical mean-field theory of strongly correlated fermion systems and the limit of infinite dimensions
journal, January 1996

  • Georges, Antoine; Kotliar, Gabriel; Krauth, Werner
  • Reviews of Modern Physics, Vol. 68, Issue 1
  • DOI: 10.1103/RevModPhys.68.13

Microscopic theory of the insulating electronic ground states of the actinide dioxides AnO 2 (An = U, Np, Pu, Am, and Cm)
journal, November 2013

NMR Evidence for the 8.5 K Phase Transition in Americium Dioxide
journal, May 2010

  • Tokunaga, Yo; Nishi, Tsuyoshi; Kambe, Shinsaku
  • Journal of the Physical Society of Japan, Vol. 79, Issue 5
  • DOI: 10.1143/JPSJ.79.053705

Self-interaction correction to density-functional approximations for many-electron systems
journal, May 1981

Structural, thermodynamic, and electronic properties of plutonium oxides from first principles
journal, August 2008

What Is the Actual Local Crystalline Structure of Uranium Dioxide, UO 2 ? A New Perspective for the Most Used Nuclear Fuel
journal, December 2016

Calculation of the magnetic anisotropy with projected-augmented-wave methodology and the case study of disordered Fe 1 x Co x alloys
journal, June 2016

Improved tetrahedron method for Brillouin-zone integrations
journal, June 1994

Magnetic excitations and dynamical Jahn-Teller distortions in UO 2
journal, June 1999

First-principles study of surface properties of PuO2: Effects of thickness and O-vacancy on surface stability and chemical activity
journal, July 2012

First-order phase transition in UO 2 : 235 U and 17 O NMR study
journal, February 2001

Actinide speciation in relation to biological processes
journal, November 2006

Density Functional Theory Studies of the Electronic Structure of Solid State Actinide Oxides
journal, October 2012

  • Wen, Xiao-Dong; Martin, Richard L.; Henderson, Thomas M.
  • Chemical Reviews, Vol. 113, Issue 2
  • DOI: 10.1021/cr300374y

Inhomogeneous Electron Gas
journal, March 1973

Voltage- and time-dependent valence state transition in cobalt oxide catalysts during the oxygen evolution reaction
journal, April 2020

Electronic Correlation and Transport Properties of Nuclear Fuel Materials
text, January 2010

Works referencing / citing this record:

Interaction of hydrogen with actinide dioxide (111) surfaces
journal, April 2019

  • Pegg, James T.; Shields, Ashley E.; Storr, Mark T.
  • The Journal of Chemical Physics, Vol. 150, Issue 13
  • DOI: 10.1063/1.5087577