Method for locating low-energy solutions within DFT+U

B. Meredig*, A. Thompson, H. A. Hansen, C. Wolverton, A. Van De Walle

*Corresponding author for this work

Research output: Contribution to journalArticle

155 Scopus citations

Abstract

The widely employed DFT+U formalism is known to give rise to many self-consistent yet energetically distinct solutions in correlated systems, which can be highly problematic for reliably predicting the thermodynamic and physical properties of such materials. Here we study this phenomenon in the bulk materials UO2, CoO, and NiO, and in a CeO2 surface. We show that the following factors affect which self-consistent solution a DFT+U calculation reaches: (i) the magnitude of U; (ii) initial correlated orbital occupations; (iii) lattice geometry; (iv) whether lattice symmetry is enforced on the charge density; and (v) even electronic mixing parameters. These various solutions may differ in total energy by hundreds of meV per atom, so identifying or approximating the ground state is critical in the DFT+U scheme. We propose an efficient U -ramping method for locating low-energy solutions, which we validate in a range of test cases. We also suggest that this method may be applicable to hybrid functional calculations.

Original languageEnglish (US)
Article number195128
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume82
Issue number19
DOIs
StatePublished - Nov 22 2010

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics

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