Magnetism and finite-temperature effects in UZr2: A density functional theory analysis

Shousha, Shehab; Beeler, Benjamin

doi:10.1016/j.jnucmat.2024.155037

Title: Magnetism and finite-temperature effects in UZr₂: A density functional theory analysis

Journal Article · 24 March 2024 · Journal of Nuclear Materials

DOI: https://doi.org/10.1016/j.jnucmat.2024.155037 · OSTI ID:2438420

^[1];

^[2]

North Carolina State University, Raleigh, NC (United States)
North Carolina State University, Raleigh, NC (United States); Idaho National Laboratory (INL), Idaho Falls, ID (United States)

The structure and the thermophysical properties of d-UZr₂ are investigated using 0 K density functional theory and ab initio molecular dynamics (AIMD). Modeling the true paramagnetic state of this intermetallic compound has been challenging using first-principles calculations. For the first time, we find that the generalized gradient approximation method without applying an on-site Coulomb interaction term (Hubbard U) can result in a ground state that is antiferromagnetic (AFM). We believe that this weak AFM ground state is the closest to the real paramagnetic state. We found that structure optimization at finite temperatures using AIMD is necessary to achieve this ground state instead of the non-magnetic and ferromagnetic states previously reported in the literature. Our findings indicate that applying the Hubbard U on uranium f-orbitals in this metallic system is unnecessary and not recommended, as it leads to a large overestimation of the volume and introduces an unphysical strong spin polarization. Finally, our approach results in atomic volume, thermal expansion, and heat capacities that have strong agreement with experiments.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC07-05ID14517; NE0009271

OSTI ID:: 2438420

Report Number(s):: INL/JOU--24-79824-Rev000

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 595; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (50)

The U-Zr (Uranium-Zirconium) system Sheldon, R. I.; Peterson, D. E. Bulletin of Alloy Phase Diagrams, Vol. 10, Issue 2 https://doi.org/10.1007/BF02881432	journal	April 1989
Heat capacities of uranium-zirconium alloys from 300 to 1100 K Takahashi, Yoichi; Yamamoto, Kazutaka; Ohsato, Tetsuo Journal of Nuclear Materials, Vol. 167 https://doi.org/10.1016/0022-3115(89)90436-4	journal	September 1989
Stability and structure of the δ phase of the U-Zr alloys Akabori, M.; Itoh, A.; Ogawa, T. Journal of Nuclear Materials, Vol. 188 https://doi.org/10.1016/0022-3115(92)90480-9	journal	June 1992
Enthalpy of formation of UZr2 by calorimetry Nagarajan, K.; Babu, R.; Mathews, C. K. Journal of Nuclear Materials, Vol. 203, Issue 3 https://doi.org/10.1016/0022-3115(93)90378-C	journal	September 1993
Free energy of formation of δ-UZr2 comment on the paper: K. Nagarajan, R. Babu and C.K. Mathews, Enthalpy of formation of UZr2 by calorimetry Ogawa, Toru Journal of Nuclear Materials, Vol. 209, Issue 1 https://doi.org/10.1016/0022-3115(94)90251-8	journal	March 1994
Thirty years of fuels and materials information from EBR-II Walters, L. C. Journal of Nuclear Materials, Vol. 270, Issue 1-2 https://doi.org/10.1016/S0022-3115(98)00760-0	journal	April 1999
The alloy theoretic automated toolkit: A user guide van de Walle, A.; Asta, M.; Ceder, G. Calphad, Vol. 26, Issue 4 https://doi.org/10.1016/S0364-5916(02)80006-2	journal	December 2002
Progress in the thermodynamic modelling of the O–U–Zr ternary system Chevalier, Pierre-Yves; Fischer, Evelyne; Cheynet, Bertrand Calphad, Vol. 28, Issue 1 https://doi.org/10.1016/j.calphad.2004.03.005	journal	March 2004
Multicomponent multisublattice alloys, nonconfigurational entropy and other additions to the Alloy Theoretic Automated Toolkit van de Walle, Axel Calphad, Vol. 33, Issue 2 https://doi.org/10.1016/j.calphad.2008.12.005	journal	June 2009
Efficient stochastic generation of special quasirandom structures van de Walle, A.; Tiwary, P.; de Jong, M. Calphad, Vol. 42 https://doi.org/10.1016/j.calphad.2013.06.006	journal	September 2013
First principles studies of hydrogen insertion effects on magnetic properties, bonding and structure reordering of UZr 2 Matar, Samir F. Computational Condensed Matter, Vol. 12 https://doi.org/10.1016/j.cocom.2017.08.001	journal	September 2017
Recent progress in simulations of the paramagnetic state of magnetic materials Abrikosov, I. A.; Ponomareva, A. V.; Steneteg, P. Current Opinion in Solid State and Materials Science, Vol. 20, Issue 2 https://doi.org/10.1016/j.cossms.2015.07.003	journal	April 2016
Density-functional study of the U–Zr system Landa, Alex; Söderlind, Per; Turchi, Patrice E. A. Journal of Alloys and Compounds, Vol. 478, Issue 1-2 https://doi.org/10.1016/j.jallcom.2008.12.052	journal	June 2009
Microstructure of α-U and δ-UZr2 phase uranium–zirconium alloys irradiated with 140-keV He+ ion-beam Ahn, Sangjoon; Irukuvarghula, Sandeep; McDeavitt, Sean M. Journal of Alloys and Compounds, Vol. 681 https://doi.org/10.1016/j.jallcom.2016.04.219	journal	October 2016
Microstructural and thermophysical properties of U–6wt.%Zr alloy for fast reactor application Kaity, Santu; Banerjee, Joydipta; Nair, M. R. Journal of Nuclear Materials, Vol. 427, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2012.03.045	journal	August 2012
First principles calculations of the structure and elastic constants of α, β and γ uranium Beeler, Benjamin; Deo, Chaitanya; Baskes, Michael Journal of Nuclear Materials, Vol. 433, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2012.09.019	journal	February 2013
Electron correlation and relativity of the 5f electrons in the U–Zr alloy system Söderlind, P.; Sadigh, B.; Lordi, V. Journal of Nuclear Materials, Vol. 444, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.10.021	journal	January 2014
Microstructural investigation of uranium rich U–Zr–Nb ternary alloy system Ghoshal, Kaushik; Kaity, Santu; Mishra, Sudhir Journal of Nuclear Materials, Vol. 446, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.12.015	journal	March 2014
Decomposition of the γ phase in as-cast and quenched U–Zr alloys Irukuvarghula, S.; Ahn, Sangjoon; McDeavitt, S. M. Journal of Nuclear Materials, Vol. 473 https://doi.org/10.1016/j.jnucmat.2016.02.028	journal	May 2016
Postirradiation examination results of several metallic fuel alloys and forms from low burnup AFC irradiations Harp, Jason M.; Chichester, Heather J. M.; Capriotti, Luca Journal of Nuclear Materials, Vol. 509 https://doi.org/10.1016/j.jnucmat.2018.07.003	journal	October 2018
Anisotropic lattice thermal expansion of uranium-based metallic fuels: A high-temperature X-ray diffraction study Park, Jeongmi; Cho, Su Yeon; Youn, Young-Sang Journal of Nuclear Materials, Vol. 527 https://doi.org/10.1016/j.jnucmat.2019.151803	journal	December 2019
Choosing the correct strong correlation correction for U3Si2: Influence of magnetism Liu, Huan; Claisse, Antoine; Middleburgh, Simon C. Journal of Nuclear Materials, Vol. 527 https://doi.org/10.1016/j.jnucmat.2019.151828	journal	December 2019
About the enthalpy of formation of the UZr2 compound Gyasi, Sandra; Benigni, Pierre; Rogez, Jacques Journal of Nuclear Materials, Vol. 562 https://doi.org/10.1016/j.jnucmat.2022.153580	journal	April 2022
Phase evolution of U-Zr system in a thermal cycling neutron diffraction experiment: as-cast U-35Zr and U-50Zr Xie, Yi; Vogel, Sven C.; Benson, Michael T. Journal of Nuclear Materials, Vol. 564 https://doi.org/10.1016/j.jnucmat.2022.153681	journal	June 2022
Finite temperature properties of uranium mononitride Kocevski, Vancho; Rehn, Daniel A.; Terricabras, Adrien J. Journal of Nuclear Materials, Vol. 576 https://doi.org/10.1016/j.jnucmat.2023.154241	journal	April 2023
Phase transformations and thermal expansion coefficients of unirradiated U-X wt.% Zr (X = 6, 10, 20, 30) measured via neutron diffraction Williams, W. J.; Vogel, S. C.; Okuniewski, M. A. Journal of Nuclear Materials, Vol. 579 https://doi.org/10.1016/j.jnucmat.2023.154380	journal	June 2023
Metallic Fuels: The EBR-II Legacy and Recent Advances Mariani, Robert D.; Porter, Douglas L.; Hayes, Steven L. Procedia Chemistry, Vol. 7 https://doi.org/10.1016/j.proche.2012.10.078	journal	January 2012
Challenges for Density Functional Theory Cohen, Aron J.; Mori-Sánchez, Paula; Yang, Weitao Chemical Reviews, Vol. 112, Issue 1 https://doi.org/10.1021/cr200107z	journal	December 2011
Adiabatic Elastic Moduli of Single Crystal Alpha‐Uranium Fisher, E. S.; McSkimin, H. J. Journal of Applied Physics, Vol. 29, Issue 10 https://doi.org/10.1063/1.1722972	journal	October 1958
Perspective on density functional theory Burke, Kieron The Journal of Chemical Physics, Vol. 136, Issue 15 https://doi.org/10.1063/1.4704546	journal	April 2012
Magnetic, transport and thermal properties of δ -phase UZr ₂ Ding, Xiaxin; Yao, Tiankai; Fu, Lyuwen Philosophical Magazine Letters, Vol. 101, Issue 1 https://doi.org/10.1080/09500839.2020.1833375	journal	November 2020
Effect of Mott-Hubbard correlations on the electronic structure and structural stability of uranium dioxide Dudarev, S. L.; Manh, D. Nguyen; Sutton, A. P. Philosophical Magazine B, Vol. 75, Issue 5 https://doi.org/10.1080/13642819708202343	journal	May 1997
First principles calculations for defects in U Beeler, B.; Good, B.; Rashkeev, S. Journal of Physics: Condensed Matter, Vol. 22, Issue 50 https://doi.org/10.1088/0953-8984/22/50/505703	journal	November 2010
The lattice stability and structure of delta -UZr ₂ at elevated temperatures Akabori, M.; Ogawa, T.; Itoh, A. Journal of Physics: Condensed Matter, Vol. 7, Issue 43 https://doi.org/10.1088/0953-8984/7/43/005	journal	October 1995
Chemical ordering as a precursor to formation of ordered δ-UZr ₂ phase: a theoretical and experimental study Ghosh, P. S.; Arya, A.; Basak, C. B. Journal of Physics: Condensed Matter, Vol. 33, Issue 25 https://doi.org/10.1088/1361-648X/abf20b	journal	May 2021
Single-Crystal Elastic Moduli and the hcp → bcc Transformation in Ti, Zr, and Hf Fisher, E. S.; Renken, C. J. Physical Review, Vol. 135, Issue 2A https://doi.org/10.1103/PhysRev.135.A482	journal	July 1964
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
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
Linear response approach to the calculation of the effective interaction parameters in the LDA + U method Cococcioni, Matteo; de Gironcoli, Stefano Physical Review B, Vol. 71, Issue 3 https://doi.org/10.1103/PhysRevB.71.035105	journal	January 2005
Oxidation energies of transition metal oxides within the GGA + U framework Wang, Lei; Maxisch, Thomas; Ceder, Gerbrand Physical Review B, Vol. 73, Issue 19 https://doi.org/10.1103/PhysRevB.73.195107	journal	May 2006
Equation of state of paramagnetic CrN from ab initio molecular dynamics Steneteg, Peter; Alling, Björn; Abrikosov, Igor A. Physical Review B, Vol. 85, Issue 14 https://doi.org/10.1103/PhysRevB.85.144404	journal	April 2012
Correlation and relativistic effects in U metal and U-Zr alloy: Validation of ab initio approaches Xie, Wei; Xiong, Wei; Marianetti, Chris A. Physical Review B, Vol. 88, Issue 23 https://doi.org/10.1103/PhysRevB.88.235128	journal	December 2013
Comment on “Correlation and relativistic effects in U metal and U-Zr alloy: Validation of ab initio approaches” Söderlind, P.; Landa, A.; Turchi, P. E. A. Physical Review B, Vol. 90, Issue 15 https://doi.org/10.1103/PhysRevB.90.157101	journal	October 2014
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
Investigation of real materials with strong electronic correlations by the LDA+DMFT method Anisimov, V. I.; Lukoyanov, A. V. Acta Crystallographica Section C Structural Chemistry, Vol. 70, Issue 2 https://doi.org/10.1107/S2053229613032312	journal	January 2014
Lightbridge Corporation’s Advanced Metallic Fuel for Light Water Reactors Malone, James; Totemeier, Aaron; Shapiro, Norton Nuclear Technology, Vol. 180, Issue 3 https://doi.org/10.13182/NT12-A15354	journal	December 2012
Determination of Thermal Expansion, Defect Formation Energy, and Defect-Induced Strain of α-U Via ab Initio Molecular Dynamics Beeler, Benjamin; Mahbuba, Khadija; Wang, Yuhao Frontiers in Materials, Vol. 8 https://doi.org/10.3389/fmats.2021.661387	journal	June 2021
High-Temperature Thermodynamics of Uranium from Ab Initio Modeling Söderlind, Per; Landa, Alexander; Moore, Emily E. Applied Sciences, Vol. 13, Issue 4 https://doi.org/10.3390/app13042123	journal	February 2023
Ground-State and Thermodynamical Properties of Uranium Mononitride from Anharmonic First-Principles Theory Söderlind, Per; Landa, Alexander; Perron, Aurélien Applied Sciences, Vol. 9, Issue 18 https://doi.org/10.3390/app9183914	journal	September 2019

Similar Records

¹⁵¹Eu Mössbauer study of magnetic ordering in flux-grown ferromagnetic and antiferromagnetic forms of EuCd₂As₂

Journal Article · 2024 · AIP Advances · OSTI ID:2294098

Ryan, D. H.; Jo, Na Hyun; Kuthanazhi, Brinda; +2 more

Inverse and normal magnetocaloric effects in LaFe{sub 12}B{sub 6}

Journal Article · 2016 · Journal of Applied Physics · OSTI ID:22596748

Diop, L. V. B.,; Isnard, O.

Interplay of electronic, magnetic, and structural properties of GdB₆ from first principles

Journal Article · 2019 · Physical Review B · OSTI ID:1613119

Xu, Shaowen; Jia, Fanhao; Yang, Yali; +4 more

Related Subjects

36 MATERIALS SCIENCE
Hubbard U
ab initio molecular dynamics
density functional theory
magnetism
metallic fuel
uranium zirconium

Title: Magnetism and finite-temperature effects in UZr2: A density functional theory analysis

Citation Formats

References (50)

Similar Records

Related Subjects

Title: Magnetism and finite-temperature effects in UZr₂: A density functional theory analysis