Ab-initio informed cluster dynamics simulation of self- and Xe diffusivity in uranium mononitride under irradiation

Schneider, Anton Jacques; Matthews, Christopher; Andersson, David Anders Ragnar; Cooper, Michael William Donald

doi:10.1016/j.jnucmat.2025.156360

Ab-initio informed cluster dynamics simulation of self- and Xe diffusivity in uranium mononitride under irradiation

Journal Article · Sun Dec 07 00:00:00 EST 2025 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2025.156360· OSTI ID:3007527

^[1]; ^[1]; ^[1]; ^[1]

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Uranium mononitride (UN) is one of the ceramic nuclear fuel alternatives to oxide fuels considered for light water reactor and advanced reactor designs, as it presents significant advantages such as high uranium density (better economics) and high thermal conductivity and melting point (increased safety). Self- and fission gas diffusivities need to be better understood, given that they influence key fuel performance phenomena like swelling and fission gas release. Recently, radiation enhanced diffusivity was investigated in UN by means of cluster dynamics simulations relying on empirical potential-based parameterizations, the reliability of which highly depends on the interatomic potential accuracy. Here, in this work, we refine this approach by determining, using ab-initio calculations, the properties of defect clusters containing vacancies, self-interstitials and Xe impurities. We also consider larger clusters than previous studies. The obtained dataset (formation enthalpies, entropies, and migration barriers) is used to parameterize a cluster dynamics model of mobile clusters, and to calculate the defect cluster concentrations under irradiation. This gives us access to the radiation enhanced self- and fission gas diffusivities. Although the resulting diffusivities are close to the values reported in the literature, we find important qualitative differences in the diffusion mechanisms. Capturing the correct mechanisms is crucial to properly describe the chemistry and fission rate dependence of the model.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: 89233218CNA000001; NE0008824

OSTI ID:: 3007527

Report Number(s):: LA-UR--25-23679; 10.1016/j.jnucmat.2025.156360

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 620; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (74)

Thermal and mechanical properties of uranium nitride prepared by SPS technique Muta, Hiroaki; Kurosaki, Ken; Uno, Masayoshi Journal of Materials Science, Vol. 43, Issue 19 https://doi.org/10.1007/s10853-008-2731-x	journal	October 2008
U + N2 Reaction layer growths Benz, Robert; Hutchinson, W. B. Journal of Nuclear Materials, Vol. 36, Issue 2 https://doi.org/10.1016/0022-3115(70)90137-6	journal	August 1970
Cation self-diffusion in UN1+x Reimann, D. K.; Kroegbr, D. M.; Lundy, T. S. Journal of Nuclear Materials, Vol. 38, Issue 2 https://doi.org/10.1016/0022-3115(71)90042-0	journal	February 1971
The distribution of intragranular fission gas bubbles in UO2 during irradiation Turnbull, J. A. Journal of Nuclear Materials, Vol. 38, Issue 2 https://doi.org/10.1016/0022-3115(71)90044-4	journal	February 1971
The effect of grain size on the swelling and gas release properties of uo2 during irradiation Turnbull, J. A. Journal of Nuclear Materials, Vol. 50, Issue 1 https://doi.org/10.1016/0022-3115(74)90061-0	journal	February 1974
Enhanced fission-product release by grain-boundary diffusion Speight, M. V.; Turnbull, J. A. Journal of Nuclear Materials, Vol. 68, Issue 2 https://doi.org/10.1016/0022-3115(77)90243-4	journal	October 1977
Swelling analysis of highly-rated MX-type LMFBR fuels: II. Microsopic swelling behaviour Ronchi, C.; Ray, I. L. F.; Thiele, H. Journal of Nuclear Materials, Vol. 74, Issue 2 https://doi.org/10.1016/0022-3115(78)90359-8	journal	June 1978
The diffusion coefficients of gaseous and volatile species during the irradiation of uranium dioxide Turnbull, J. A.; Friskney, C. A.; Findlay, J. R. Journal of Nuclear Materials, Vol. 107, Issue 2-3 https://doi.org/10.1016/0022-3115(82)90419-6	journal	June 1982
Local fission gas release and swelling in water reactor fuel during slow power transients Mogensen, M.; Walker, C. T.; Ray, I. L. F. Journal of Nuclear Materials, Vol. 131, Issue 2-3 https://doi.org/10.1016/0022-3115(85)90455-6	journal	April 1985
Formation energies of helium-void complexes in nickel Adams, J. B.; Wolfer, W. G. Journal of Nuclear Materials, Vol. 166, Issue 3 https://doi.org/10.1016/0022-3115(89)90220-1	journal	August 1989
Material property correlations for uranium mononitride Hayes, S. L.; Thomas, J. K.; Peddicord, K. L. Journal of Nuclear Materials, Vol. 171, Issue 2-3 https://doi.org/10.1016/0022-3115(90)90375-W	journal	May 1990
Formation and growth of intragranular fission gas bubbles in UO2 fuels with burnup of 6–83 GWd/t Kashibe, S.; Une, K.; Nogita, K. Journal of Nuclear Materials, Vol. 206, Issue 1 https://doi.org/10.1016/0022-3115(93)90229-R	journal	November 1993
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
Point Defects and Transport Properties in Carbides and Nitrides Matzke, Hj. Studies in Inorganic Chemistry https://doi.org/10.1016/B978-0-444-88534-0.50018-7	book	December 1988
Temperature dependency of dislocation evolution in Kr-irradiated Uranium mononitride (UN) through in-situ TEM observation and modeling Kosmidou, Maria; Matthews, Christopher; Terricabras, Adrien J. Acta Materialia, Vol. 288 https://doi.org/10.1016/j.actamat.2025.120824	journal	April 2025
The diffusion of point defects in uranium mononitride: Combination of DFT and atomistic simulation with novel potential Kuksin, A. Yu.; Starikov, S. V.; Smirnova, D. E. Journal of Alloys and Compounds, Vol. 658 https://doi.org/10.1016/j.jallcom.2015.10.223	journal	February 2016
The development of grain-face porosity in irradiated oxide fuel White, R. J. Journal of Nuclear Materials, Vol. 325, Issue 1 https://doi.org/10.1016/j.jnucmat.2003.10.008	journal	February 2004
A molecular dynamics study of radiation induced diffusion in uranium dioxide Martin, G.; Maillard, S.; Brutzel, L. Van Journal of Nuclear Materials, Vol. 385, Issue 2 https://doi.org/10.1016/j.jnucmat.2008.12.010	journal	March 2009
Implementing first principles calculations of defect migration in a fuel performance code for UN simulations Kotomin, E. A.; Mastrikov, Yu. A.; Rashkeev, S. N. Journal of Nuclear Materials, Vol. 393, Issue 2 https://doi.org/10.1016/j.jnucmat.2009.06.016	journal	September 2009
Atomistic modeling of intrinsic and radiation-enhanced fission gas (Xe) diffusion in UO2±x: Implications for nuclear fuel performance modeling Andersson, D. A.; Garcia, P.; Liu, X. -Y. Journal of Nuclear Materials, Vol. 451, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.03.041	journal	August 2014
Uncertainty and sensitivity analysis of fission gas behavior in engineering-scale fuel modeling Pastore, Giovanni; Swiler, L. P.; Hales, J. D. Journal of Nuclear Materials, Vol. 456 https://doi.org/10.1016/j.jnucmat.2014.09.077	journal	January 2015
GGA+U study of uranium mononitride: A comparison of the U-ramping and occupation matrix schemes and incorporation energies of fission products Claisse, Antoine; Klipfel, Marco; Lindbom, Niclas Journal of Nuclear Materials, Vol. 478 https://doi.org/10.1016/j.jnucmat.2016.06.007	journal	September 2016
Ab-initio study of C and O impurities in uranium nitride Lopes, Denise Adorno; Claisse, Antoine; Olsson, Pär Journal of Nuclear Materials, Vol. 478 https://doi.org/10.1016/j.jnucmat.2016.06.008	journal	September 2016
Simulation of radiation driven fission gas diffusion in UO2, ThO2 and PuO2 Cooper, M. W. D.; Stanek, C. R.; Turnbull, J. A. Journal of Nuclear Materials, Vol. 481 https://doi.org/10.1016/j.jnucmat.2016.09.013	journal	December 2016
First-principles study of water reacting with the (110) surface of uranium mononitride Bo, Tao; Lan, Jian-Hui; Zhao, Yao-Lin Journal of Nuclear Materials, Vol. 492 https://doi.org/10.1016/j.jnucmat.2017.05.026	journal	August 2017
A model describing intra-granular fission gas behaviour in oxide fuel for advanced engineering tools Pizzocri, D.; Pastore, G.; Barani, T. Journal of Nuclear Materials, Vol. 502 https://doi.org/10.1016/j.jnucmat.2018.02.024	journal	April 2018
Unit mechanisms of fission gas release: Current understanding and future needs Tonks, Michael; Andersson, David; Devanathan, Ram Journal of Nuclear Materials, Vol. 504 https://doi.org/10.1016/j.jnucmat.2018.03.016	journal	June 2018
Fission gas release from UO2 nuclear fuel: A review Rest, J.; Cooper, M. W. D.; Spino, J. Journal of Nuclear Materials, Vol. 513 https://doi.org/10.1016/j.jnucmat.2018.08.019	journal	January 2019
Description of phase transitions through accumulation of point defects: UN, UO2 and UC Starikov, S.; Korneva, M. Journal of Nuclear Materials, Vol. 510 https://doi.org/10.1016/j.jnucmat.2018.08.025	journal	November 2018
Atomistic modeling of out-of-pile xenon diffusion by vacancy clusters in UO2 Perriot, Romain; Matthews, Christopher; Cooper, Michael W. D. Journal of Nuclear Materials, Vol. 520 https://doi.org/10.1016/j.jnucmat.2019.03.050	journal	July 2019
Application of SPS in the fabrication of UN and (U,Th)N pellets from microspheres Gonzalez Fonseca, L. G.; Hedberg, M.; Huan, L. Journal of Nuclear Materials, Vol. 536 https://doi.org/10.1016/j.jnucmat.2020.152181	journal	August 2020
Modeling intra-granular fission gas bubble evolution and coarsening in uranium dioxide during in-pile transients Barani, T.; Pastore, G.; Magni, A. Journal of Nuclear Materials, Vol. 538 https://doi.org/10.1016/j.jnucmat.2020.152195	journal	September 2020
Cluster dynamics simulation of xenon diffusion during irradiation in UO2 Matthews, Christopher; Perriot, Romain; Cooper, M. W. D. Journal of Nuclear Materials, Vol. 540 https://doi.org/10.1016/j.jnucmat.2020.152326	journal	November 2020
Radiation driven diffusion in γU-Mo Beeler, Benjamin; Cooper, Michael W. D.; Mei, Zhi-Gang Journal of Nuclear Materials, Vol. 543 https://doi.org/10.1016/j.jnucmat.2020.152568	journal	January 2021
Improvement of the BISON U 3 Si 2 modeling capabilities based on multiscale developments to modeling fission gas behavior Gamble, K. A.; Pastore, G.; Cooper, M. W. D. Journal of Nuclear Materials, Vol. 555 https://doi.org/10.1016/j.jnucmat.2021.153097	journal	November 2021
Irradiation-enhanced diffusion and diffusion-limited creep in U3Si2 Cooper, M. W. D.; Gamble, K. A.; Capolungo, L. Journal of Nuclear Materials, Vol. 555 https://doi.org/10.1016/j.jnucmat.2021.153129	journal	November 2021
Dislocation Loops in Proton Irradiated Uranium-Nitrogen-Oxygen System Xiu, Pengyuan; Jin, Miaomiao; Bawane, Kaustubh Journal of Nuclear Materials, Vol. 557 https://doi.org/10.1016/j.jnucmat.2021.153244	journal	December 2021
First-principles investigation of uranium mononitride (UN): Effect of magnetic ordering, spin-orbit interactions and exchange correlation functional Kocevski, Vancho; Rehn, Daniel A.; Cooper, Michael W. D. Journal of Nuclear Materials, Vol. 559 https://doi.org/10.1016/j.jnucmat.2021.153401	journal	February 2022
Atomistic and cluster dynamics modeling of fission gas (Xe) diffusivity in TRISO fuel kernels Liu, X. -Y.; Matthews, C.; Jiang, W. Journal of Nuclear Materials, Vol. 561 https://doi.org/10.1016/j.jnucmat.2022.153539	journal	April 2022
Development and application of a uranium mononitride (UN) potential: Thermomechanical properties and Xe diffusion Kocevski, Vancho; Cooper, Michael W. D.; Claisse, Antoine J. Journal of Nuclear Materials, Vol. 562 https://doi.org/10.1016/j.jnucmat.2022.153553	journal	April 2022
Diffusion of krypton and xenon in uranium mononitride; a Density Functional Theory Study Yang, Lin; Kaltsoyannis, Nikolas Journal of Nuclear Materials, Vol. 566 https://doi.org/10.1016/j.jnucmat.2022.153803	journal	August 2022
Simulations of self- and Xe diffusivity in uranium mononitride including chemistry and irradiation effects Cooper, M. W. D.; Rizk, J.; Matthews, C. Journal of Nuclear Materials, Vol. 587 https://doi.org/10.1016/j.jnucmat.2023.154685	journal	December 2023
Radiation induced athermal diffusivity in uranium mononitride Schneider, Anton; Rizk, Jason; Kosmidou, Maria Journal of Nuclear Materials, Vol. 601 https://doi.org/10.1016/j.jnucmat.2024.155313	journal	December 2024
The role of irradiation-enhanced interstitial diffusion in over-pressurizing fission gas bubbles in UO2 Cooper, M. W. D.; Matthews, C.; Andersson, D. A. Journal of Nuclear Materials, Vol. 604 https://doi.org/10.1016/j.jnucmat.2024.155452	journal	January 2025
Physics-based modelling of fission gas swelling and release in UO2 applied to integral fuel rod analysis Pastore, Giovanni; Luzzi, Lelio; Di Marcello, Valentino Nuclear Engineering and Design, Vol. 256 https://doi.org/10.1016/j.nucengdes.2012.12.002	journal	March 2013
Incorporation of Kr and Xe in Uranium Mononitride: A Density Functional Theory Study Yang, Lin; Kaltsoyannis, Nikolas The Journal of Physical Chemistry C, Vol. 125, Issue 48 https://doi.org/10.1021/acs.jpcc.1c08523	journal	November 2021
Oxygen Potential, Uranium Diffusion, and Defect Chemistry in UO_2±x: A Density Functional Theory Study Neilson, William D.; Rizk, Jason; Cooper, Michael W. D. The Journal of Physical Chemistry C, Vol. 128, Issue 50 https://doi.org/10.1021/acs.jpcc.4c06580	journal	December 2024
Some Phase Equilibria in the Uranium-Nitrogen System ¹ Benz, R.; Bowman, M. G. Journal of the American Chemical Society, Vol. 88, Issue 2 https://doi.org/10.1021/ja00954a015	journal	January 1966
A Screened Hybrid DFT Study of Actinide Oxides, Nitrides, and Carbides Wen, Xiao-Dong; Martin, Richard L.; Scuseria, Gustavo E. The Journal of Physical Chemistry C, Vol. 117, Issue 25 https://doi.org/10.1021/jp403141t	journal	June 2013
Atomic mechanisms of mass transport in ceramic nuclear fuel materials Matzke, Hansjoachim Journal of the Chemical Society, Faraday Transactions, Vol. 86, Issue 8 https://doi.org/10.1039/ft9908601243	journal	January 1990
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
The effect of the Perdew-Zunger self-interaction correction to density functionals on the energetics of small molecules Klüpfel, Simon; Klüpfel, Peter; Jónsson, Hannes The Journal of Chemical Physics, Vol. 137, Issue 12 https://doi.org/10.1063/1.4752229	journal	September 2012
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
On the theory of impurity diffusion in metals Le Claire, A. D. The Philosophical Magazine: A Journal of Theoretical Experimental and Applied Physics, Vol. 7, Issue 73 https://doi.org/10.1080/14786436208201866	journal	January 1962
Swelling in UO ₂ under conditions of gas release Turnbull, J. A.; Tucker, M. O. Philosophical Magazine, Vol. 30, Issue 1 https://doi.org/10.1080/14786439808206532	journal	July 1974
Special points for Brillouin-zone integrations Monkhorst, Hendrik J.; Pack, James D. Physical Review B, Vol. 13, Issue 12, p. 5188-5192 https://doi.org/10.1103/PhysRevB.13.5188	journal	June 1976
Nature of the 5 f electrons in uranium nitride: A photoelectron spectroscopic study of UN, U, U O 2 , ThN, and Th Norton, P. R.; Tapping, R. L.; Creber, D. K. Physical Review B, Vol. 21, Issue 6 https://doi.org/10.1103/PhysRevB.21.2572	journal	March 1980
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
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
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
First-principles calculations of uranium diffusion in uranium dioxide Dorado, Boris; Andersson, David A.; Stanek, Christopher R. Physical Review B, Vol. 86, Issue 3 https://doi.org/10.1103/PhysRevB.86.035110	journal	July 2012
Itinerant nature of U 5 f states in uranium mononitride revealed by angle-resolved photoelectron spectroscopy Fujimori, Shin-ichi; Ohkochi, Takuo; Okane, Tetsuo Physical Review B, Vol. 86, Issue 23 https://doi.org/10.1103/PhysRevB.86.235108	journal	December 2012
Point defect modeling in materials: Coupling ab initio and elasticity approaches Varvenne, Céline; Bruneval, Fabien; Marinica, Mihai-Cosmin Physical Review B, Vol. 88, Issue 13 https://doi.org/10.1103/PhysRevB.88.134102	journal	October 2013
Transport properties in dilute UN ( X ) solid solutions ( X = Xe , Kr ) Claisse, Antoine; Schuler, Thomas; Lopes, Denise Adorno Physical Review B, Vol. 94, Issue 17 https://doi.org/10.1103/PhysRevB.94.174302	journal	November 2016
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
Nitrogen Diffusion in Uranium Nitride as Measured by Alpha Particle Activation of 15N Holt, J. B.; Almassy, Marcia Y. Journal of the American Ceramic Society, Vol. 52, Issue 12 https://doi.org/10.1111/j.1151-2916.1969.tb16064.x	journal	December 1969
THE OXIDATION OF NIAL: What Can We Learn from Ab Initio Calculations? Finnis, M. W.; Lozovoi, A. Y.; Alavi, A. Annual Review of Materials Research, Vol. 35, Issue 1 https://doi.org/10.1146/annurev.matsci.35.101503.091652	journal	August 2005
A Calculation on the Migration of Fission Gas in Material Exhibiting Precipitation and Re-solution of Gas Atoms Under Irradiation Speight, M. V. Nuclear Science and Engineering, Vol. 37, Issue 2 https://doi.org/10.13182/NSE69-A20676	journal	August 1969
Impact of Accident-Tolerant Fuels and Claddings on the Overall Fuel Cycle: A Preliminary Systems Analysis Youinou, Gilles J.; Sen, R. Sonat Nuclear Technology, Vol. 188, Issue 2 https://doi.org/10.13182/NT14-22	journal	November 2014
The Sodium-Bonding Pin Concept for Advanced Fuels Part I: Swelling of Carbide Fuel up to 12% Burnup Colin, Michel; Coquerelle, Michel; Ray, Ian L. F. Nuclear Technology, Vol. 63, Issue 3 https://doi.org/10.13182/NT83-A33271	journal	December 1983
Notizen: Xe-133 Diffusion in UN Single Crystals Oi, Noboru Zeitschrift für Naturforschung A, Vol. 21, Issue 6 https://doi.org/10.1515/zna-1966-0641	journal	January 1966
Examination of the impact of electron–phonon coupling on fission enhanced diffusion in uranium dioxide using classical molecular dynamics Wormald, Jonathan L.; Hawari, Ayman I. Journal of Materials Research, Vol. 30, Issue 9 https://doi.org/10.1557/jmr.2014.405	journal	February 2015
First-principles Phonon Calculations with Phonopy and Phono3py Togo, Atsushi Journal of the Physical Society of Japan, Vol. 92, Issue 1 https://doi.org/10.7566/JPSJ.92.012001	journal	January 2023

Similar Records

Radiation induced athermal diffusivity in uranium mononitride

Journal Article · Sun Aug 04 20:00:00 EDT 2024 · Journal of Nuclear Materials · OSTI ID:2429291

Simulations of self- and Xe diffusivity in uranium mononitride including chemistry and irradiation effects

Journal Article · Sun Aug 27 20:00:00 EDT 2023 · Journal of Nuclear Materials · OSTI ID:1998128

Development and application of a uranium mononitride (UN) potential: Thermomechanical properties and Xe diffusion

Journal Article · Tue Feb 01 19:00:00 EST 2022 · Journal of Nuclear Materials · OSTI ID:1845260

Related Subjects

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
36 MATERIALS SCIENCE

Ab-initio informed cluster dynamics simulation of self- and Xe diffusivity in uranium mononitride under irradiation

Citation Formats

References (74)

Similar Records

Related Subjects