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Noncollinear Relativistic DFT + U Calculations of Actinide Dioxide Surfaces

  • James T. Pegg*
    James T. Pegg
    Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, U.K.
    Atomic Weapons Establishment (AWE) Plc, Aldermaston, Reading RG7 4PR, U.K.
    *E-mail: [email protected]
  • Ashley E. Shields
    Ashley E. Shields
    Oak Ridge National Laboratory, One Bethel Valley Road, Oak Ridge, Tennessee 37831, United States
  • Mark T. Storr
    Mark T. Storr
    Atomic Weapons Establishment (AWE) Plc, Aldermaston, Reading RG7 4PR, U.K.
  • David O. Scanlon
    David O. Scanlon
    Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, U.K.
    Diamond Light Source Ltd., Diamond House, Harwell Science and Innovation Campus, Didcot, Oxfordshire OX11 0DE, U.K.
    Thomas Young Centre, University College London, Gower Street, London WC1E 6BT, U.K.
  • , and 
  • Nora H. de Leeuw
    Nora H. de Leeuw
    Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, U.K.
    School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff CF1D 3AT, U.K.
Cite this: J. Phys. Chem. C 2019, 123, 1, 356–366
Publication Date (Web):December 6, 2018
https://doi.org/10.1021/acs.jpcc.8b07823
Copyright © 2018 American Chemical Society

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    Abstract

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    A noncollinear relativistic PBEsol + U study of low-index actinide dioxides (AnO2, An = U, Np, or Pu) surfaces has been conducted. The importance of magnetic vector reorientation relative to the plane of the surface is highlighted; this has often been ignored in collinear nonrelativistic models. The use of noncollinear relativistic methods is key to the design of reliable computational models. The ionic relaxation of each surface is shown to be confined to the first three monolayers, and we have explored the configurations of the terminal oxygen ions on the reconstructed (001) surface. The reconstructed (001) surfaces are ordered as (001)αβ < (001)α < (001)β in terms of energetics. Electrostatic potential isosurface and scanning tunneling microscopy images have also been calculated. By considering the energetics of the low-index AnO2 surfaces, an octahedral Wulff crystal morphology has been calculated.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.8b07823.

    • Monolayer surface energetics, fixed unit cell dimensions, initial magnetic structure, structural ionic relaxation, and magnetic deviation (PDF)

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    Cited By

    This article is cited by 15 publications.

    1. Justin G. Terhorst, Theodore A. Corcovilos, Michael J. van Stipdonk. Conversion of a UO22+ Precursor to UH+ and U+ Using Tandem Mass Spectrometry to Remove Both “yl” Oxo Ligands. Journal of the American Society for Mass Spectrometry 2023, 34 (11) , 2439-2442. https://doi.org/10.1021/jasms.3c00260
    2. Eric Hoar, Thomas C. Shehee, Lindsay E. Roy. Impact of Precipitation Parameters on the Specific Surface Area of PuO2. ACS Omega 2022, 7 (1) , 540-547. https://doi.org/10.1021/acsomega.1c04964
    3. Bingyun Ao. Atom-Resolved Chemical States in the Multivalent U-TM-O (TM: Ti, V, Cr, Mn, Fe, Ni, Nb, Mo, W) Ternary Oxides from First-Principles. The Journal of Physical Chemistry C 2019, 123 (49) , 29609-29622. https://doi.org/10.1021/acs.jpcc.9b09523
    4. Binod K Rai, Alex Bretaña, Gregory Morrison, Rosalie Greer, Krzysztof Gofryk, Hans-Conrad zur Loye. Crystal structure and magnetism of actinide oxides: a review. Reports on Progress in Physics 2024, 87 (6) , 066501. https://doi.org/10.1088/1361-6633/ad38cb
    5. Amanda R. Bubas, Irena J. Tatosian, Anna Iacovino, Theodore A. Corcovilos, Michael J. van Stipdonk. Reactions of gas-phase uranyl formate/acetate anions: reduction of carboxylate ligands to aldehydes by intra-complex hydride attack. Physical Chemistry Chemical Physics 2024, 26 (16) , 12753-12763. https://doi.org/10.1039/D4CP00823E
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    7. Luke J. Metzler, Christopher T. Farmen, Theodore A. Corcovilos, Michael J. Van Stipdonk. Intrinsic chemistry of [OUCH] + : reactions with H 2 O, CH 3 CN and O 2. Physical Chemistry Chemical Physics 2021, 23 (8) , 4475-4479. https://doi.org/10.1039/D1CP00177A
    8. Huiying Gao, Menglei Li, Yu Yang, Ping Zhang. First-principles calculation of structural, magnetic and electronic properties of PuO2-H , 0≤x≤2. Journal of Alloys and Compounds 2021, 857 , 157592. https://doi.org/10.1016/j.jallcom.2020.157592
    9. James T. Pegg, Ashley E. Shields, Mark T. Storr, David O. Scanlon, Nora H. de Leeuw. Interaction of hydrogen with actinide dioxide (011) surfaces. The Journal of Chemical Physics 2020, 153 (1) https://doi.org/10.1063/5.0010200
    10. Samuel Moxon, Adam R. Symington, Joshua S. Tse, James Dawson, Joseph M. Flitcroft, Stephen C. Parker, David J. Cooke, Robert M. Harker, Marco Molinari. The energetics of carbonated PuO 2 surfaces affects nanoparticle morphology: a DFT+ U study. Physical Chemistry Chemical Physics 2020, 22 (15) , 7728-7737. https://doi.org/10.1039/D0CP00021C
    11. Jonathan Collard, Helen Steele, Nikolas Kaltsoyannis. Computational study of HCl adsorption on stoichiometric and oxygen vacancy PuO2 {111}, {110} and {100} surfaces. Journal of Nuclear Materials 2020, 530 , 151951. https://doi.org/10.1016/j.jnucmat.2019.151951
    12. E. Torres, T.P. Kaloni. Thermal conductivity and diffusion mechanisms of noble gases in uranium dioxide: A DFT+U study. Journal of Nuclear Materials 2019, 521 , 137-145. https://doi.org/10.1016/j.jnucmat.2019.04.040
    13. S. L. Dudarev, P. Liu, D. A. Andersson, C. R. Stanek, T. Ozaki, C. Franchini. Parametrization of LSDA + U for noncollinear magnetic configurations: Multipolar magnetism in UO 2 . Physical Review Materials 2019, 3 (8) https://doi.org/10.1103/PhysRevMaterials.3.083802
    14. James T. Pegg, Ashley E. Shields, Mark T. Storr, David O. Scanlon, Nora H. de Leeuw. Interaction of hydrogen with actinide dioxide (111) surfaces. The Journal of Chemical Physics 2019, 150 (13) https://doi.org/10.1063/1.5087577
    15. James T. Pegg, Ashley E. Shields, Mark T. Storr, Andrew S. Wills, David O. Scanlon, Nora H. de Leeuw. Magnetic structure of UO 2 and NpO 2 by first-principle methods. Physical Chemistry Chemical Physics 2019, 21 (2) , 760-771. https://doi.org/10.1039/C8CP03581D