The Dirac equation in electronic structure calculations: Accurate evaluation of DFT predictions for actinides
- Los Alamos National Laboratory
- Sandia National Laboratories
Brooks, Johansson, and Skriver, using the LMTO-ASA method and considerable insight, were able to explain many of the ground state properties of the actinides. In the many years since this work was done, electronic structure calculations of increasing sophistication have been applied to actinide elements and compounds, attempting to quantify the applicability of DFT to actinides and actinide compounds and to try to incorporate other methodologies (i.e. DMFT) into DFT calculations. Through these calculations, the limits of both available density functionals and ad hoc methodologies are starting to become clear. However, it has also become clear that approximations used to incorporate relativity are not adequate to provide rigorous tests of the underlying equations of DFT, not to mention ad hoc additions. In this talk, we describe the result of full-potential LMTO calculations for the elemental actinides, comparing results obtained with a full Dirac basis with those obtained from scalar-relativistic bases, with and without variational spin-orbit. This comparison shows that the scalar relativistic treatment of actinides does not have sufficient accuracy to provide a rigorous test of theory and that variational spin-orbit introduces uncontrolled errors in the results of electronic structure calculations on actinide elements.
- Research Organization:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Organization:
- DOE/LANL
- DOE Contract Number:
- AC52-06NA25396
- OSTI ID:
- 1043027
- Report Number(s):
- LA-UR-12-21972; TRN: US1202992
- Resource Relation:
- Conference: Electronic structure theory for materials modeling: from early days to current success. ; 2012-06-10 - 2012-06-11 ; Stockholm, Sweden
- Country of Publication:
- United States
- Language:
- English
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