Exploring metastable states in UO2 using hybrid functionals and dynamical mean field theory

Ratcliff, Laura E.; Genovese, Luigi; Park, Hyowon; Littlewood, Peter B.; Lopez-Bezanilla, Alejandro

doi:10.1088/1361-648x/ac3cf1

Title: Exploring metastable states in UO₂ using hybrid functionals and dynamical mean field theory

Journal Article · 15 December 2021 · Journal of Physics. Condensed Matter

DOI: https://doi.org/10.1088/1361-648x/ac3cf1 · OSTI ID:1846919

^[1];

^[2]; Park, Hyowon ^[3]; Littlewood, Peter B. ^[4];

^[5]

Imperial College London (United Kingdom)
Alternative Energies and Atomic Energy Commission (CEA), Grenoble (France). INAC-SP2m; Univ. Grenoble Alpes (France)
Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Illinois, Chicago, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Chicago, IL (United States). James Franck Inst.
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

A detailed exploration of the f-atomic orbital occupancy space for UO2 is performed using a first principles approach based on density functional theory (DFT), employing a full hybrid functional within a systematic basis set. Specifically, the PBE0 functional is combined with an occupancy biasing scheme implemented in a wavelet-based algorithm which is adapted to large supercells. The results are compared with previous DFT + U calculations reported in the literature, while dynamical mean field theory is also performed to provide a further base for comparison. This work shows that the computational complexity of the energy landscape of a correlated f-electron oxide is much richer than has previously been demonstrated. The resulting calculations provide evidence of the existence of multiple previously unexplored metastable electronic states of UO₂, including those with energies which are lower than previously reported ground states.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; EPSRC; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1846919

Report Number(s):: LA-UR-21-30127

Journal Information:: Journal of Physics. Condensed Matter, Journal Name: Journal of Physics. Condensed Matter Journal Issue: 9 Vol. 34; ISSN 0953-8984

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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