The Conundrum of Relaxation Volumes in First-Principles Calculations of Charged Defects in UO2

Goyal, Anuj; Mathew, Kiran; Hennig, Richard G.; Chernatynskiy, Aleksandr; Stanek, Christopher R.; Murphy, Samuel T.; Andersson, David A.; Phillpot, Simon R.; Uberuaga, Blas P.

doi:10.3390/app9245276

Title: The Conundrum of Relaxation Volumes in First-Principles Calculations of Charged Defects in UO2

Journal Article · Wed Dec 04 00:00:00 EST 2019 · Applied Sciences

DOI:https://doi.org/10.3390/app9245276· OSTI ID:1577208

Goyal, Anuj; Mathew, Kiran; Hennig, Richard G.; Chernatynskiy, Aleksandr; Stanek, Christopher R.;

; Andersson, David A.; Phillpot, Simon R.; Uberuaga, Blas P.

The defect relaxation volumes obtained from density-functional theory (DFT) calculations of charged vacancies and interstitials are much larger than their neutral counterparts, seemingly unphysically large. We focus on UO₂ as our primary material of interest, but also consider Si and GaAs to reveal the generality of our results. In this work, we investigate the possible reasons for this and revisit the methods that address the calculation of charged defects in periodic DFT. We probe the dependence of the proposed energy corrections to charged defect formation energies on relaxation volumes and find that corrections such as potential alignment remain ambiguous with regards to its contribution to the charged defect relaxation volume. We also investigate the volume for the net neutral defect reactions comprising individual charged defects, and find that the aggregate formation volumes have reasonable magnitudes. This work highlights the issue that, as is well-known for defect formation energies, the defect formation volumes depend on the choice of reservoir. We show that considering the change in volume of the electron reservoir in the formation reaction of the charged defects, analogous to how volumes of atoms are accounted for in defect formation volumes, can renormalize the formation volumes of charged defects such that they are comparable to neutral defects. This approach enables the description of the elastic properties of isolated charged defects within an overall neutral material.

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

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: 10-2258; Nuclear Energy Advanced Modeling and Simulations; 89233218CNA000001

OSTI ID:: 1577208

Alternate ID(s):: OSTI ID: 1597330

Report Number(s):: LA-UR-17-22816; ASPCC7; PII: app9245276

Journal Information:: Applied Sciences, Journal Name: Applied Sciences Vol. 9 Journal Issue: 24; ISSN 2076-3417

Publisher:: MDPICopyright Statement

Country of Publication:: Switzerland

Language:: English

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Cited by: 9 works

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Title: The Conundrum of Relaxation Volumes in First-Principles Calculations of Charged Defects in UO2

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