10.1021/acs.jpcc.8b07823.s001
James T. Pegg
James T.
Pegg
Ashley E. Shields
Ashley E.
Shields
Mark T. Storr
Mark T.
Storr
David O. Scanlon
David O.
Scanlon
Nora H. de Leeuw
Nora
H. de Leeuw
Noncollinear Relativistic DFT + <i>U</i> Calculations of
Actinide Dioxide Surfaces
American Chemical Society
2018
low-index AnO 2 surfaces
octahedral Wulff crystal morphology
U Calculations
low-index actinide dioxides
Actinide Dioxide Surfaces
vector reorientation
terminal oxygen ions
AnO 2
Noncollinear Relativistic DFT
U study
collinear nonrelativistic models
scanning tunneling microscopy images
2018-12-06 00:00:00
Journal contribution
https://acs.figshare.com/articles/journal_contribution/Noncollinear_Relativistic_DFT_i_U_i_Calculations_of_Actinide_Dioxide_Surfaces/7520090
A noncollinear
relativistic PBEsol + <i>U</i> study of
low-index actinide dioxides (AnO<sub>2</sub>, 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
AnO<sub>2</sub> surfaces, an octahedral Wulff crystal morphology has
been calculated.