Pegg, JT;
Shields, AE;
Storr, MT;
Scanlon, DO;
De Leeuw, NH;
(2019)
Noncollinear Relativistic DFT + U Calculations of Actinide Dioxide Surfaces.
Journal of Physical Chemistry C
, 123
(1)
pp. 356-366.
10.1021/acs.jpcc.8b07823.
Preview |
Text
Pegg_AAM_Noncollinear Relativistic DFT+U Calculations of Actinide Dioxide Surfaces(FinalMain) (1).pdf - Accepted Version Download (2MB) | Preview |
Preview |
Text
Pegg_AAMSup_Noncollinear Relativistic DFT+U Calculations of Actinide Dioxide Surfaces (FinalSupporting Information).pdf - Accepted Version Download (577kB) | Preview |
Abstract
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.
| Type: | Article |
|---|---|
| Title: | Noncollinear Relativistic DFT + U Calculations of Actinide Dioxide Surfaces |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acs.jpcc.8b07823 |
| Publisher version: | https://doi.org/10.1021/acs.jpcc.8b07823 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10066733 |
Archive Staff Only
 |
View Item |
