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.