Density functional theory study of defects in unalloyed δ-Pu

Hernandez, S. C.; Freibert, F. J.; Wills, J. M.

doi:10.1016/j.scriptamat.2017.02.025

Title: Density functional theory study of defects in unalloyed δ-Pu

Journal Article · 19 March 2017 · Scripta Materialia

DOI: https://doi.org/10.1016/j.scriptamat.2017.02.025 · OSTI ID:1357125

Hernandez, S. C. ^[1]; Freibert, F. J. ^[1]; Wills, J. M. ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Using density functional theory, we explore in this paper various classical point and complex defects within the face-centered cubic unalloyed δ-plutonium matrix that are potentially induced from self-irradiation. For plutonium only defects, the most energetically stable defect is a distorted split-interstitial. Gallium, the δ-phase stabilizer, is thermodynamically stable as a substitutional defect, but becomes unstable when participating in a complex defect configuration. Finally, complex uranium defects may thermodynamically exist as uranium substitutional with neighboring plutonium interstitial and stabilization of uranium within the lattice is shown via partial density of states and charge density difference plots to be 5f hybridization between uranium and plutonium.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Los Alamos National Laboratory (LANL)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1357125

Report Number(s):: LA-UR-16-29243

Journal Information:: Scripta Materialia, Journal Name: Scripta Materialia Vol. 134; ISSN 1359-6462

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (41)

Introduction to modeling and simulations of plutonium aging Schwartz, Adam J.; Wolfer, Wilhelm G. Journal of Computer-Aided Materials Design, Vol. 14, Issue 3 https://doi.org/10.1007/s10820-007-9055-z	journal	July 2007
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Thermodynamic, alloying and defect properties of plutonium: Density-functional calculations Robert, G.; Pasturel, A.; Siberchicot, B. Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2006.09.118	journal	October 2007
Analysis of density changes in plutonium observed from accelerated aging using Pu-238 enrichment Chung, Brandon W.; Saw, Cheng K.; Thompson, Stephen R. Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2006.10.017	journal	October 2007
Formation and recovery of irradiation and mechanical damage in stabilized δ-plutonium alloys Freibert, F. J.; Dooley, D. E.; Miller, D. A. Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2006.10.051	journal	October 2007
Simulations of low energy cascades in fcc Pu metal at 300 K and constant volume Valone, Steven M.; Baskes, Michael I.; Stan, Marius Journal of Nuclear Materials, Vol. 324, Issue 1 https://doi.org/10.1016/j.jnucmat.2003.09.006	journal	January 2004
Volume changes in δ-plutonium from helium and other decay products Wolfer, W. G.; Söderlind, Per; Landa, A. Journal of Nuclear Materials, Vol. 355, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2006.03.018	journal	September 2006
Study by XRD of the lattice swelling of PuGa alloys induced by self-irradiation Ravat, B.; Oudot, B.; Baclet, N. Journal of Nuclear Materials, Vol. 366, Issue 1-2 https://doi.org/10.1016/j.jnucmat.2007.02.003	journal	June 2007
A plutonium α-decay defects production study through displacement cascade simulations with MEAM potential Berlu, L.; Jomard, G.; Rosa, G. Journal of Nuclear Materials, Vol. 374, Issue 3 https://doi.org/10.1016/j.jnucmat.2007.09.012	journal	March 2008
Point defect formation and migration in Ga stabilised δ-Pu Robinson, M.; Kenny, S. D.; Smith, R. Journal of Nuclear Materials, Vol. 423, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2011.11.046	journal	April 2012
He migration and bubble formation in Ga stabilised δ-Pu Robinson, M.; Kenny, S. D.; Smith, R. Journal of Nuclear Materials, Vol. 444, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.10.017	journal	January 2014
Theoretical confirmation of Ga-stabilized anti-ferromagnetism in plutonium metal Söderlind, Per; Landa, Alex Journal of Nuclear Materials, Vol. 448, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.02.017	journal	May 2014
Thermodynamic re-assessment of the Pu–U system and its application to the ternary Pu–U–Ga system Perron, A.; Turchi, P. E. A.; Landa, A. Journal of Nuclear Materials, Vol. 454, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.07.051	journal	November 2014
Effects of self-irradiation in plutonium alloys Chung, B. W.; Lema, K. E.; Allen, P. G. Journal of Nuclear Materials, Vol. 471 https://doi.org/10.1016/j.jnucmat.2015.09.028	journal	April 2016
Simulating radiation damage in δ-plutonium Robinson, M.; Kenny, S. D.; Smith, R. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 267, Issue 18 https://doi.org/10.1016/j.nimb.2009.06.113	journal	September 2009
Phonon and magnetic structure in δ-plutonium from density-functional theory Söderlind, Per; Zhou, F.; Landa, A. Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep15958	journal	October 2015
First-principles calculations for defects and impurities: Applications to III-nitrides Van de Walle, Chris G.; Neugebauer, Jörg Journal of Applied Physics, Vol. 95, Issue 8 https://doi.org/10.1063/1.1682673	journal	April 2004
Isochronal annealing effects on local structure, crystalline fraction, and undamaged region size of radiation damage in Ga-stabilized δ -Pu Olive, D. T.; Wang, D. L.; Booth, C. H. Journal of Applied Physics, Vol. 120, Issue 3 https://doi.org/10.1063/1.4958856	journal	July 2016
The Big Science of stockpile stewardship Reis, Victor H.; Hanrahan, Robert J.; Levedahl, W. Kirk Physics Today, Vol. 69, Issue 8 https://doi.org/10.1063/PT.3.3268	journal	August 2016
Emergent magnetic moments produced by self-damage in plutonium McCall, S. K.; Fluss, M. J.; Chung, B. W. Proceedings of the National Academy of Sciences, Vol. 103, Issue 46 https://doi.org/10.1073/pnas.0608552103	journal	November 2006
Origin of the multiple configurations that drive the response of δ-plutonium’s elastic moduli to temperature Migliori, Albert; Söderlind, Per; Landa, Alexander Proceedings of the National Academy of Sciences, Vol. 113, Issue 40 https://doi.org/10.1073/pnas.1609215113	journal	September 2016
Ab initio study of gallium stabilized δ-plutonium alloys and hydrogen–vacancy complexes Hernandez, Sarah C.; Schwartz, Daniel S.; Taylor, Christopher D. Journal of Physics: Condensed Matter, Vol. 26, Issue 23 https://doi.org/10.1088/0953-8984/26/23/235502	journal	May 2014
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/PhysRevB.49.14251	journal	May 1994
Short-range atomic structure of 1 wt. % Ga δ-stabilized plutonium by x-ray-absorption fine-structure spectroscopy Cox, L. E.; Martinez, R.; Nickel, J. H. Physical Review B, Vol. 51, Issue 2 https://doi.org/10.1103/PhysRevB.51.751	journal	January 1995
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Simple model for complex structures Söderlind, Per; Wills, J. M.; Eriksson, O. Physical Review B, Vol. 57, Issue 3 https://doi.org/10.1103/PhysRevB.57.1320	journal	January 1998
Vibrational properties of Ga-stabilized δ − Pu by extended x-ray absorption fine structure Allen, P. G.; Henderson, A. L.; Sylwester, E. R. Physical Review B, Vol. 65, Issue 21 https://doi.org/10.1103/PhysRevB.65.214107	journal	June 2002
First-principles elastic and structural properties of uranium metal Söderlind, Per Physical Review B, Vol. 66, Issue 8 https://doi.org/10.1103/PhysRevB.66.085113	journal	August 2002
Density-functional investigation of magnetism in δ -Pu Söderlind, Per; Landa, Alex; Sadigh, Babak Physical Review B, Vol. 66, Issue 20 https://doi.org/10.1103/PhysRevB.66.205109	journal	November 2002
First-principles elastic constants and phonons of δ ‐ Pu Söderlind, P.; Landa, A.; Sadigh, B. Physical Review B, Vol. 70, Issue 14 https://doi.org/10.1103/PhysRevB.70.144103	journal	October 2004
Absence of magnetic moments in plutonium Lashley, J. C.; Lawson, A.; McQueeney, R. J. Physical Review B, Vol. 72, Issue 5 https://doi.org/10.1103/PhysRevB.72.054416	journal	August 2005
Competition between delocalization and spin-orbit splitting in the actinide 5 f states Tobin, J. G.; Moore, K. T.; Chung, B. W. Physical Review B, Vol. 72, Issue 8 https://doi.org/10.1103/PhysRevB.72.085109	journal	August 2005
Gallium stabilization of δ − Pu : Density-functional calculations Sadigh, Babak; Wolfer, Wilhelm G. Physical Review B, Vol. 72, Issue 20 https://doi.org/10.1103/PhysRevB.72.205122	journal	November 2005
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)] Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 78, Issue 7 https://doi.org/10.1103/PhysRevLett.78.1396	journal	February 1997
First-principles calculations for point defects in solids Freysoldt, Christoph; Grabowski, Blazej; Hickel, Tilmann Reviews of Modern Physics, Vol. 86, Issue 1 https://doi.org/10.1103/RevModPhys.86.253	journal	March 2014
Structure of ζ-phase plutonium–uranium Lawson, A. C.; Goldstone, J. A.; Cort, B. Acta Crystallographica Section B Structural Science, Vol. 52, Issue 1 https://doi.org/10.1107/S0108768195006811	journal	February 1996
The valence-fluctuating ground state of plutonium Janoschek, Marc; Das, Pinaki; Chakrabarti, Bismayan Science Advances, Vol. 1, Issue 6 https://doi.org/10.1126/sciadv.1500188	journal	July 2015
Vacancy formation in δ-plutonium: A density-functional study in the generalized gradient approximation Robert, G.; Pasturel, A.; Siberchicot, B. Europhysics Letters (EPL), Vol. 71, Issue 3 https://doi.org/10.1209/epl/i2005-10094-2	journal	August 2005
Computational modeling of actinide materials and complexes Söderlind, Per; Kotliar, G.; Haule, K. MRS Bulletin, Vol. 35, Issue 11 https://doi.org/10.1557/mrs2010.715	journal	November 2010

Cited By (1)

Density-functional theory for plutonium Söderlind, Per; Landa, A.; Sadigh, B. Advances in Physics, Vol. 68, Issue 1 https://doi.org/10.1080/00018732.2019.1599554	journal	January 2019

Similar Records

Ab initio study of the effects of dilute defects on the local structure of unalloyed δ-plutonium

Technical Report · 2016 · OSTI ID:1334088

Hernandez, Sarah Christine; Kisiel, Elliot Steven; Freibert, Franz Joseph

Investigating the Role of Defects in α-Pu Phase Transitions using Density Functional Theory

Technical Report · 2023 · OSTI ID:1972168

Boden, Samuel Bishop

Spin density stabilization of local distortions induced by a monovacancy in

δ

-Pu

Journal Article · 2018 · Physical Review Materials · OSTI ID:1483534

Hernandez, Sarah C.; Freibert, Franz J.; Hoagland, Richard G.; +2 more

Related Subjects

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Complex defects
Delta-plutonium
Density functional theory
Point defects

Title: Density functional theory study of defects in unalloyed δ-Pu

Citation Formats

References (41)

Cited By (1)

Similar Records

Related Subjects