Ab initio prediction of rapid kinetics of Fe impurities in δ-Pu

Kweon, Kyoung E.; Söderlind, Per; Sadigh, Babak

doi:10.1116/6.0004600

Ab initio prediction of rapid kinetics of Fe impurities in δ-Pu

Journal Article · Fri Jun 20 00:00:00 EDT 2025 · Journal of Vacuum Science & Technology A

DOI:https://doi.org/10.1116/6.0004600· OSTI ID:2587884

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Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Here, we study the formation energies of iron impurities in δ-Pu within spin–orbital-polarized density functional theory (SOP-DFT). The thermodynamic solubility limit of iron in δ-Pu is calculated, indicating low miscibility. We show that surprisingly, Fe impurities at equilibrium are almost equally likely to occupy octahedral interstitial sites or substitutional sites, with slight preference for the former. In contrast, we find the energy of the tetrahedral interstitial Fe to be nearly 1 eV higher than the octahedral one. We explore the energy landscape for Fe impurity hopping diffusion and conclude that Fe impurities in δ-Pu are divided into two populations: (i) Immobile substitutional Fe impurities and (ii) highly mobile interstitial Fe impurities. The latter, (ii), migrate between octahedral interstitial sites with an energy barrier of around 0.2 eV. The energy barrier for exchange between the two populations is calculated to exceed 0.7 eV. Finally, we discuss the role of magnetic order on the impurity energetics.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 2587884

Report Number(s):: LLNL--JRNL-2003969

Journal Information:: Journal of Vacuum Science & Technology A, Journal Name: Journal of Vacuum Science & Technology A Journal Issue: 4 Vol. 43; ISSN 1520-8559; ISSN 0734-2101

Publisher:: American Vacuum SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Ab initio prediction of rapid kinetics of Fe impurities in δ-Pu

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