Electronic structure and thermodynamic approaches to the prospect of super abundant vacancies in δ-Pu

Muñoz, Alexander; Matanovic, Ivana; Gifford, Brendan; Rudin, Sven; Holland, Troy; Jones, Travis

doi:10.1039/D4CP00534A

Title: Electronic structure and thermodynamic approaches to the prospect of super abundant vacancies in δ-Pu

Journal Article · 24 April 2024 · Physical Chemistry Chemical Physics. PCCP

DOI: https://doi.org/10.1039/D4CP00534A · OSTI ID:2335979

^[1];

^[1]; Gifford, Brendan ^[1]; Rudin, Sven ^[1]; Holland, Troy ^[1]; Jones, Travis ^[1]

T-1: Physics and Chemistry of Materials, Theoretical Division, Los Alamos National Laboratory, Los Alamos, NM 87545, USA

In this manuscript, we use density functional theory to develop thermodynamic models for super abundant vacancy (SAV) formation in delta-Pu. We find that the formation of a hydride phase will occur before reaching the H pressures needed to form a SAV phase.

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Sponsoring Organization:: USDOE

OSTI ID:: 2335979

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 16 Vol. 26; ISSN 1463-9076; ISSN PPCPFQ

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

References (38)

Uncertainty quantification in thermochemistry, benchmarking electronic structure computations, and Active Thermochemical Tables Ruscic, Branko International Journal of Quantum Chemistry, Vol. 114, Issue 17 https://doi.org/10.1002/qua.24605	journal	January 2014
Crystal Structure of Delta-Prime Plutonium And the Thermal Expansion Characteristics Of Delta, Delta-Prime, and Epsilon Plutonium Ellinger, F. H. JOM, Vol. 8, Issue 10 https://doi.org/10.1007/BF03377861	journal	October 1956
The variation of lattice parameter with hydrogen content of non-stoichiometric plutonium dihydride Muromura, T.; Yahata, T.; Ouchi, K. Journal of Inorganic and Nuclear Chemistry, Vol. 34, Issue 1 https://doi.org/10.1016/0022-1902(72)80375-0	journal	January 1972
Formation of superabundant vacancies in metal hydrides at high temperatures Fukai, Yuh Journal of Alloys and Compounds, Vol. 231, Issue 1-2 https://doi.org/10.1016/0925-8388(95)01834-4	journal	December 1995
Superabundant vacancy–hydrogen clusters in electrodeposited Ni and Cu Fukai, Y.; Mizutani, M.; Yokota, S. Journal of Alloys and Compounds, Vol. 356-357 https://doi.org/10.1016/S0925-8388(02)01270-7	journal	August 2003
Vacancy formation energies in metals: A comparison of MetaGGA with LDA and GGA exchange–correlation functionals Medasani, Bharat; Haranczyk, Maciej; Canning, Andrew Computational Materials Science, Vol. 101 https://doi.org/10.1016/j.commatsci.2015.01.018	journal	April 2015
Structural, magnetic, and dynamic properties of PuH2+ (x= 0, 0.25, 0.5, 0.75, 1): A hybrid density functional study Li, Shichang; Guo, Yong; Ye, Xiaoqiu International Journal of Hydrogen Energy, Vol. 42, Issue 52 https://doi.org/10.1016/j.ijhydene.2017.11.011	journal	December 2017
Symmetry-correct bonding in density functional theory calculations for delta phase Pu Rudin, Sven P. Journal of Nuclear Materials, Vol. 570 https://doi.org/10.1016/j.jnucmat.2022.153954	journal	November 2022
A density functional study of atomic hydrogen adsorption on plutonium layers Huda, M. N.; Ray, A. K. Physica B: Condensed Matter, Vol. 352, Issue 1-4 https://doi.org/10.1016/j.physb.2004.06.010	journal	October 2004
A benchmark database for adsorption bond energies to transition metal surfaces and comparison to selected DFT functionals Wellendorff, Jess; Silbaugh, Trent L.; Garcia-Pintos, Delfina Surface Science, Vol. 640 https://doi.org/10.1016/j.susc.2015.03.023	journal	October 2015
Jacob’s Ladder as Sketched by Escher: Assessing the Performance of Broadly Used Density Functionals on Transition Metal Surface Properties Vega, Lorena; Ruvireta, Judit; Viñes, Francesc Journal of Chemical Theory and Computation, Vol. 14, Issue 1 https://doi.org/10.1021/acs.jctc.7b01047	journal	December 2017
Quantum Accurate Prediction of Plutonium–Plutonium Dihydride Phase Equilibrium Using a Lattice Gas Model Mullen, Ryan Gotchy; Goldman, Nir The Journal of Physical Chemistry C, Vol. 124, Issue 38 https://doi.org/10.1021/acs.jpcc.0c04869	journal	August 2020
Establishing the Accuracy of Broadly Used Density Functionals in Describing Bulk Properties of Transition Metals Janthon, Patanachai; Kozlov, Sergey M.; Viñes, Francesc Journal of Chemical Theory and Computation, Vol. 9, Issue 3 https://doi.org/10.1021/ct3010326	journal	February 2013
The Plutonium-Hydrogen System. I. Plutonium Dihydride and Dideuteride ¹ Mulford, Robert N. R.; Sturdy, Gladys E. Journal of the American Chemical Society, Vol. 77, Issue 13 https://doi.org/10.1021/ja01618a005	journal	July 1955
First-Principles Study of Superabundant Vacancy Formation in Metal Hydrides Zhang, Changjun; Alavi, Ali Journal of the American Chemical Society, Vol. 127, Issue 27 https://doi.org/10.1021/ja050475w	journal	July 2005
Effects of Concentration, Crystal Structure, Magnetism, and Electronic Structure Method on First-Principles Oxygen Vacancy Formation Energy Trends in Perovskites Curnan, Matthew T.; Kitchin, John R. The Journal of Physical Chemistry C, Vol. 118, Issue 49 https://doi.org/10.1021/jp507957n	journal	November 2014
Hidden magnetic order in plutonium dioxide nuclear fuel Pegg, James T.; Shields, Ashley E.; Storr, Mark T. Physical Chemistry Chemical Physics, Vol. 20, Issue 32 https://doi.org/10.1039/C8CP03583K	journal	January 2018
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points Henkelman, Graeme; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22 https://doi.org/10.1063/1.1323224	journal	December 2000
A climbing image nudged elastic band method for finding saddle points and minimum energy paths Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904 https://doi.org/10.1063/1.1329672	journal	December 2000
Theory of Positron Annihilation in Helium-Filled Bubbles in Plutonium Sterne, P. A. AIP Conference Proceedings https://doi.org/10.1063/1.1594605	conference	January 2003
Experimental Vibrational Zero-Point Energies: Diatomic Molecules Irikura, Karl K. Journal of Physical and Chemical Reference Data, Vol. 36, Issue 2 https://doi.org/10.1063/1.2436891	journal	June 2007
Detecting low concentrations of plutonium hydride with magnetization measurements Kim, Jae Wook; Mun, E. D.; Baiardo, J. P. Journal of Applied Physics, Vol. 117, Issue 5 https://doi.org/10.1063/1.4907216	journal	February 2015
A first-principles study of hydrogen surface coverage on δ-Pu (100), (111), and (110) surfaces Mullen, Ryan Gotchy; Goldman, Nir The Journal of Chemical Physics, Vol. 155, Issue 23 https://doi.org/10.1063/5.0064515	journal	December 2021
The solubility of hydrogen and deuterium in alloyed, unalloyed and impure plutonium metal Richmond, S.; Bridgewater, J. S.; Ward, J. W. IOP Conference Series: Materials Science and Engineering, Vol. 9 https://doi.org/10.1088/1757-899X/9/1/012036	journal	March 2010
Measurements of Equilibrium Vacancy Concentrations in Aluminum Simmons, R. O.; Balluffi, R. W. Physical Review, Vol. 117, Issue 1 https://doi.org/10.1103/PhysRev.117.52	journal	January 1960
High-precision sampling for Brillouin-zone integration in metals Methfessel, M.; Paxton, A. T. Physical Review B, Vol. 40, Issue 6 https://doi.org/10.1103/PhysRevB.40.3616	journal	August 1989
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
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
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Ab initio study of H-vacancy interactions in fcc metals: Implications for the formation of superabundant vacancies Nazarov, R.; Hickel, T.; Neugebauer, J. Physical Review B, Vol. 89, Issue 14 https://doi.org/10.1103/PhysRevB.89.144108	journal	April 2014
Thermodynamics, structure, and charge state of hydrogen-vacancy complexes in δ-plutonium Taylor, Christopher D.; Francis, Michael F.; Schwartz, Daniel S. Physical Review B, Vol. 89, Issue 21 https://doi.org/10.1103/PhysRevB.89.214114	journal	June 2014
Formation of Superabundant Vacancies in Pd Hydride under High Hydrogen Pressures Fukai, Yuk; Ōkuma, Nobuyuki Physical Review Letters, Vol. 73, Issue 12 https://doi.org/10.1103/PhysRevLett.73.1640	journal	September 1994
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
Spin density stabilization of local distortions induced by a monovacancy in δ -Pu Hernandez, Sarah C.; Freibert, Franz J.; Hoagland, Richard G. Physical Review Materials, Vol. 2, Issue 8 https://doi.org/10.1103/PhysRevMaterials.2.085005	journal	August 2018
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data Momma, Koichi; Izumi, Fujio Journal of Applied Crystallography, Vol. 44, Issue 6 https://doi.org/10.1107/S0021889811038970	journal	October 2011
Superabundant Vacancies Formed in MetalHydrogen Alloys Fukai, Y. Physica Scripta, Vol. T103, Issue 1 https://doi.org/10.1238/Physica.Topical.103a00011	journal	January 2003
Hydrogen-Vacancy Effects in Pu-2 at. % Ga Alloys Schwartz, Daniel S.; Richmond, Scott; Smith, Alice I. MRS Proceedings, Vol. 1444 https://doi.org/10.1557/opl.2012.1125	journal	January 2012
Structure and Properties of Cubic PuH2 and PuH3: A Density Functional Theory Study Smith, Thomas; Moxon, Samuel; Cooke, David J. Crystals, Vol. 12, Issue 10 https://doi.org/10.3390/cryst12101499	journal	October 2022

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