Molecular dynamics study of grain boundaries as defect sinks under irradiation in LiAlO2 and LiAl5O8

Roy, Ankit; Jiang, Weilin; Nandipati, Giridhar; Casella, Andrew M.; Senor, David J.; Soulami, Ayoub; Devanathan, Ram

doi:10.1038/s41529-025-00565-y

Molecular dynamics study of grain boundaries as defect sinks under irradiation in LiAlO₂ and LiAl₅O₈

Journal Article · Thu Feb 27 00:00:00 EST 2025 · npj Materials Degradation

DOI:https://doi.org/10.1038/s41529-025-00565-y· OSTI ID:2565344

Roy, Ankit ^[1]; ^[1]; ^[1]; ^[1]; Senor, David J. ^[1]; ^[1]; ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Lithium aluminate ceramics, LiAlO₂ and LiAl₅O₈, show promise in nuclear environments due to their excellent radiation tolerance. Molecular dynamics simulations investigate grain boundaries (GB) and their role in defect evolution. Results reveal that GBs act as efficient defect sinks, with Li and Al atoms exhibiting distinct behaviors during displacement cascades. Tritium migration in LiAlO₂ is also studied, showing rapid diffusion and stable configurations with oxygen, corroborated by ab initio simulations from the literature. The calculated tritium diffusion coefficient of 1.33 × 10^-¹⁴ m²/s aligns with the literature, validating the model. LiAl₅O₈ demonstrates superior defect healing compared to LiAlO₂, attributed to enhanced atomic transfer between grains and GBs. These findings reveal key insights into defect dynamics, providing essential insights for their application in tritium-producing burnable absorber rods (TPBARs).

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

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

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2565344

Report Number(s):: PNNL-SA--202853

Journal Information:: npj Materials Degradation, Journal Name: npj Materials Degradation Journal Issue: 1 Vol. 9; ISSN 2397-2106

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

References (62)

Formation of vacancy-type dislocation loops in tungsten bombarded by 60 keV Au ions Jäger, W.; Wilkens, M. Physica Status Solidi (a), Vol. 32, Issue 1 https://doi.org/10.1002/pssa.2210320109	journal	November 1975
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Dynamical simulations of displacement cascades near symmetrical tilt grain boundaries in UO2 Tian, X. F.; Gao, T.; Xiao, H. X. Indian Journal of Physics, Vol. 88, Issue 2 https://doi.org/10.1007/s12648-013-0400-7	journal	September 2013
Lithium diffusion in γ-LiAlO2, a molecular dynamics simulation Jacobs, Jean-Paul; San Miguel, Miguel Angel; Alvarez, Luis Javier Journal of Nuclear Materials, Vol. 232, Issue 2-3 https://doi.org/10.1016/S0022-3115(96)00435-7	journal	September 1996
Preferential damage at symmetrical tilt grain boundaries in bcc iron Pérez-Pérez, F. Javier; Smith, Roger Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 180, Issue 1-4 https://doi.org/10.1016/S0168-583X(01)00439-6	journal	June 2001
Stacking fault tetrahedra formation in the neighbourhood of grain boundaries Samaras, M.; Derlet, P. M.; Van Swygenhoven, H. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 202 https://doi.org/10.1016/S0168-583X(02)01829-3	journal	April 2003
Structural changes at grain boundaries in bcc iron induced by atomic collisions Pérez-Pérez, F. Javier; Smith, Roger Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 164-165 https://doi.org/10.1016/S0168-583X(99)01141-6	journal	April 2000
Survey of computed grain boundary properties in face-centered cubic metals: I. Grain boundary energy Olmsted, David L.; Foiles, Stephen M.; Holm, Elizabeth A. Acta Materialia, Vol. 57, Issue 13 https://doi.org/10.1016/j.actamat.2009.04.007	journal	August 2009
Survey of computed grain boundary properties in face-centered cubic metals—II: Grain boundary mobility Olmsted, David L.; Holm, Elizabeth A.; Foiles, Stephen M. Acta Materialia, Vol. 57, Issue 13 https://doi.org/10.1016/j.actamat.2009.04.015	journal	August 2009
Grain boundary properties of elemental metals Zheng, Hui; Li, Xiang-Guo; Tran, Richard Acta Materialia, Vol. 186 https://doi.org/10.1016/j.actamat.2019.12.030	journal	March 2020
Atomistic simulations to reveal HIP-bonding mechanisms of Al6061/Al6061 Roy, Ankit; Kalsar, Rajib; Song, Miao Acta Materialia, Vol. 281 https://doi.org/10.1016/j.actamat.2024.120402	journal	December 2024
Atomistic simulations of the interaction between transmutation-produced Re and grain boundaries in tungsten Liu, Lixia; Chen, Yangchun; Gao, Ning Computational Materials Science, Vol. 173 https://doi.org/10.1016/j.commatsci.2019.109412	journal	February 2020
Atomsk: A tool for manipulating and converting atomic data files Hirel, Pierre Computer Physics Communications, Vol. 197 https://doi.org/10.1016/j.cpc.2015.07.012	journal	December 2015
Irradiation-induced large bubble formation and grain growth in super nano-grained ceramic Zhang, Yutong; Huang, Zhangyi; Qi, Jianqi Journal of the European Ceramic Society, Vol. 41, Issue 15 https://doi.org/10.1016/j.jeurceramsoc.2021.08.051	journal	December 2021
Atomic scale modelling of the primary damage state of irradiated fcc and bcc nanocrystalline metals Samaras, M.; Derlet, P. M.; Swygenhoven, H. Van Journal of Nuclear Materials, Vol. 351, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2006.02.030	journal	June 2006
Final steps to an all tungsten divertor tokamak Neu, R.; Bobkov, V.; Dux, R. Journal of Nuclear Materials, Vol. 363-365 https://doi.org/10.1016/j.jnucmat.2006.12.021	journal	June 2007
Grain boundary influence on displacement cascades in UO2: A molecular dynamics study Brutzel, L. Van; Vincent-Aublant, E. Journal of Nuclear Materials, Vol. 377, Issue 3 https://doi.org/10.1016/j.jnucmat.2008.04.010	journal	July 2008
Derivation of potential model for LiAlO2 by simple and effective optimization of model parameters Tsuchihira, H.; Oda, T.; Tanaka, S. Journal of Nuclear Materials, Vol. 395, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2009.10.041	journal	December 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
Molecular dynamics study of fission gas bubble nucleation in UO2 Liu, X. -Y.; Andersson, D. A. Journal of Nuclear Materials, Vol. 462 https://doi.org/10.1016/j.jnucmat.2015.03.030	journal	July 2015
Molecular dynamics modeling of atomic displacement cascades in 3C–SiC: Comparison of interatomic potentials Samolyuk, G. D.; Osetsky, Y. N.; Stoller, R. E. Journal of Nuclear Materials, Vol. 465 https://doi.org/10.1016/j.jnucmat.2015.05.036	journal	October 2015
Tritium species diffusion on and desorption from γ-LiAlO2 (100) surface: A first-principles investigation Jia, Ting; Senor, David J.; Duan, Yuhua Journal of Nuclear Materials, Vol. 540 https://doi.org/10.1016/j.jnucmat.2020.152394	journal	November 2020
Molecular dynamic simulations of displacement cascades in tungsten and tungsten–rhenium alloys: Effects of grain boundary and/or σ phase Liu, Lixia; Chen, Yangchun; Gao, Ning Journal of Nuclear Materials, Vol. 561 https://doi.org/10.1016/j.jnucmat.2022.153543	journal	April 2022
Molecular dynamics simulations of radiation response of LiAlO2 and LiAl5O8 Roy, Ankit; Senor, David J.; Casella, Andrew M. Journal of Nuclear Materials, Vol. 576 https://doi.org/10.1016/j.jnucmat.2023.154280	journal	April 2023
Insights into radiation resistance of titanium alloys from displacement cascade simulations Roy, Ankit; Senor, David J.; Edwards, Danny J. Journal of Nuclear Materials, Vol. 586 https://doi.org/10.1016/j.jnucmat.2023.154695	journal	December 2023
Microstructural and compositional evolutions in γ-LiAlO2 pellets during ion irradiation at an elevated temperature Jiang, Weilin; Kovarik, Libor; Wirth, Mark G. Journal of Nuclear Materials, Vol. 591 https://doi.org/10.1016/j.jnucmat.2024.154925	journal	April 2024
Cluster dynamics simulations of tritium and helium diffusion in lithium ceramics Roy, Ankit; Sassi, Michel; Pitike, Krishna Chaitanya Journal of Nuclear Materials, Vol. 592 https://doi.org/10.1016/j.jnucmat.2024.154970	journal	April 2024
Large molecular dynamics simulations of collision cascades in single-crystal, bi-crystal, and poly-crystal UO2 Van Brutzel, L.; Vincent-Aublant, E.; Delaye, J. -M. 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.2009.06.078	journal	September 2009
Core configuration of a gas-cooled reactor as a tritium production device for fusion reactor Nakaya, H.; Matsuura, H.; Nakao, Y. Nuclear Engineering and Design, Vol. 271 https://doi.org/10.1016/j.nucengdes.2013.12.023	journal	May 2014
Energetic driving force for preferential binding of self-interstitial atoms to Fe grain boundaries over vacancies Tschopp, M. A.; Horstemeyer, M. F.; Gao, F. Scripta Materialia, Vol. 64, Issue 9 https://doi.org/10.1016/j.scriptamat.2011.01.031	journal	May 2011
Comprehensive Analysis of Hydrogen, Deuterium, Tritium and Isotopic Ratios of Other Light Elements in Neutron Irradiated TPBAR Components Devaraj, Arun; Matthews, Bethany; Arey, Bruce Microscopy and Microanalysis, Vol. 25, Issue S2 https://doi.org/10.1017/S1431927619002137	journal	August 2019
Unravelling Ultraslow Lithium-Ion Diffusion in γ-LiAlO ₂ : Experiments with Tracers, Neutrons, and Charge Carriers Wiedemann, Dennis; Nakhal, Suliman; Rahn, Johanna Chemistry of Materials, Vol. 28, Issue 3 https://doi.org/10.1021/acs.chemmater.5b04608	journal	January 2016
First-Principles Study of Tritium Trapping in γ-LiAlO₂ Nanovoids Sassi, Michel; Spurgeon, Steven R.; Matthews, Bethany E. The Journal of Physical Chemistry C, Vol. 126, Issue 12 https://doi.org/10.1021/acs.jpcc.2c00381	journal	March 2022
Insights on Amorphization of Lithium Aluminate from Atomistic Simulation Setyawan, Wahyu; Senor, David J.; Devanathan, Ram The Journal of Physical Chemistry C, Vol. 121, Issue 14 https://doi.org/10.1021/acs.jpcc.6b12562	journal	March 2017
Interstitial Lithium Diffusion Pathways in γ-LiAlO ₂ : A Computational Study Islam, Mazharul M.; Bredow, Thomas The Journal of Physical Chemistry Letters, Vol. 6, Issue 22 https://doi.org/10.1021/acs.jpclett.5b01780	journal	October 2015
ReaxFF: A Reactive Force Field for Hydrocarbons van Duin, Adri C. T.; Dasgupta, Siddharth; Lorant, Francois The Journal of Physical Chemistry A, Vol. 105, Issue 41 https://doi.org/10.1021/jp004368u	journal	October 2001
Improving atomic displacement and replacement calculations with physically realistic damage models Nordlund, Kai; Zinkle, Steven J.; Sand, Andrea E. Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-03415-5	journal	March 2018
Molecular dynamics simulations of displacement cascades in LiAlO2 and LiAl5O8 ceramics Roy, Ankit; Casella, Andrew M.; Senor, David J. Scientific Reports, Vol. 14, Issue 1 https://doi.org/10.1038/s41598-024-51222-4	journal	January 2024
Radiation Tolerance of Nanocrystalline Ceramics: Insights from Yttria Stabilized Zirconia Dey, Sanchita; Drazin, John W.; Wang, Yongqiang Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep07746	journal	January 2015
LiAl ₅ O ₈ as a potential coating material in lithium-ion batteries: a first principles study Mo, Sijia; Zhang, Bingkai; Zhang, Kecheng Physical Chemistry Chemical Physics, Vol. 21, Issue 25 https://doi.org/10.1039/C9CP02650A	journal	January 2019
A broken-bond model for grain boundaries in face-centered cubic metals Wolf, D. Journal of Applied Physics, Vol. 68, Issue 7 https://doi.org/10.1063/1.346373	journal	October 1990
Mechanism for transient migration of xenon in UO2 Liu, X. -Y.; Uberuaga, B. P.; Andersson, D. A. Applied Physics Letters, Vol. 98, Issue 15 https://doi.org/10.1063/1.3579198	journal	April 2011
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy APL Materials, Vol. 1, Issue 1 https://doi.org/10.1063/1.4812323	journal	July 2013
Microstructural evolution and precipitation in γ-LiAlO₂ during ion irradiation Jiang, Weilin; Kovarik, Libor; Zhu, Zihua Journal of Applied Physics, Vol. 131, Issue 21 https://doi.org/10.1063/5.0089865	journal	June 2022
Radiation damage near grain boundaries Samaras, M.; Derlet, P. M.; Van Swygenhoven†, H. Philosophical Magazine, Vol. 83, Issue 31-34 https://doi.org/10.1080/14786430310001600222	journal	October 2003
Multi-timescale investigation of radiation damage near TiO ₂ rutile grain boundaries Bai, Xian-Ming; Uberuaga, Blas P. Philosophical Magazine, Vol. 92, Issue 12 https://doi.org/10.1080/14786435.2011.648229	journal	April 2012
Plasma-material interactions in current tokamaks and their implications for next step fusion reactors Federici, G.; Skinner, C. H.; Brooks, J. N. Nuclear Fusion, Vol. 41, Issue 12 https://doi.org/10.1088/0029-5515/41/12/218	journal	December 2001
A reactive force field for lithium–aluminum silicates with applications to eucryptite phases Narayanan, Badri; van Duin, Adri C. T.; Kappes, Branden B. Modelling and Simulation in Materials Science and Engineering, Vol. 20, Issue 1 https://doi.org/10.1088/0965-0393/20/1/015002	journal	November 2011
Large-scale machine-learning molecular dynamics simulation of primary radiation damage in tungsten Liu, Jiahui; Byggmästar, Jesper; Fan, Zheyong Physical Review B, Vol. 108, Issue 5 https://doi.org/10.1103/PhysRevB.108.054312	journal	August 2023
Grain growth and phase stability of nanocrystalline cubic zirconia under ion irradiation Zhang, Yanwen; Jiang, Weilin; Wang, Chongmin Physical Review B, Vol. 82, Issue 18 https://doi.org/10.1103/PhysRevB.82.184105	journal	November 2010
Mechanism of Radiation Damage Reduction in Equiatomic Multicomponent Single Phase Alloys Granberg, F.; Nordlund, K.; Ullah, Mohammad W. Physical Review Letters, Vol. 116, Issue 13 https://doi.org/10.1103/PhysRevLett.116.135504	journal	April 2016
Computer Simulation of Displacement Cascades in Nanocrystalline Ni Samaras, M.; Derlet, P. M.; Van Swygenhoven, H. Physical Review Letters, Vol. 88, Issue 12 https://doi.org/10.1103/PhysRevLett.88.125505	journal	March 2002
The crystal structure and anomalous dispersion of γ-LiAlO ₂ Marezio, M. Acta Crystallographica, Vol. 19, Issue 3 https://doi.org/10.1107/S0365110X65003511	journal	September 1965
Low‐temperature crystallization of MgSiO₃ glasses under electron irradiation: Possible implications for silicate dust evolution in circumstellar environments Carrez, Philippe; Demyk, Karine; Leroux, Hugues Meteoritics & Planetary Science, Vol. 37, Issue 11 https://doi.org/10.1111/j.1945-5100.2002.tb00815.x	journal	November 2002
Role of interfaces in damage process of irradiated lithium aluminate nanocrystals Setyawan, Wahyu; Senor, David J.; Devanathan, Ram Journal of the American Ceramic Society https://doi.org/10.1111/jace.16051	journal	September 2018
Efficient Annealing of Radiation Damage Near Grain Boundaries via Interstitial Emission Bai, X. M.; Voter, A. F.; Hoagland, R. G. Science, Vol. 327, Issue 5973 https://doi.org/10.1126/science.1183723	journal	March 2010
Radiation Defects in Aluminum. Simulation of Primary Damage in Surface Collision Cascades Voskoboinikov, R. E. Physics of Metals and Metallography, Vol. 120, Issue 1 https://doi.org/10.1134/S0031918X1901006X	journal	January 2019
Simulation of Primary Radiation Damage in Nickel Voskoboinikov, R. E. Physics of Metals and Metallography, Vol. 121, Issue 1 https://doi.org/10.1134/S0031918X20010196	journal	January 2020
Computer Simulation of Displacement Damage Cascade Formation near Sigma 5 Twist Boundary in Silver Sugio, Kenjiro; Shimomura, Yoshiharu; Rubia, Tomas D. de la Journal of the Physical Society of Japan, Vol. 67, Issue 3 https://doi.org/10.1143/JPSJ.67.882	journal	March 1998
The influence of ∑3 twin boundaries on the formation of radiation-induced defect clusters in nanotwinned Cu Demkowicz, Michael J.; Anderoglu, Osman; Zhang, Xinghang Journal of Materials Research, Vol. 26, Issue 14 https://doi.org/10.1557/jmr.2011.56	journal	June 2011
Recommendations for Tritium Science and Technology Research and Development in Support of the Tritium Readiness Campaign, TTP-7-084 Senor, David J. https://doi.org/10.2172/1113608	report	October 2013
Atomistic Simulations of the Defect Chemistry and Self-Diffusion of Li-ion in LiAlO2 Kuganathan, N.; Dark, J.; Sgourou, E. N. Energies, Vol. 12, Issue 15 https://doi.org/10.3390/en12152895	journal	July 2019

Similar Records

Microstructure-dependent rate theory model of defect segregation and phase stability in irradiated polycrystalline LiAlO₂

Journal Article · Mon Dec 20 19:00:00 EST 2021 · Modelling and Simulation in Materials Science and Engineering · OSTI ID:1915261

Effect of Mg and Ni impurities on tritium diffusion in lithium ceramics through cluster dynamics simulations

Journal Article · Tue Mar 04 19:00:00 EST 2025 · Journal of Nuclear Materials · OSTI ID:2588696

Cluster dynamics simulations of tritium and helium diffusion in lithium ceramics

Journal Article · Thu Feb 15 19:00:00 EST 2024 · Journal of Nuclear Materials · OSTI ID:2406926

Related Subjects

36 MATERIALS SCIENCE

Molecular dynamics study of grain boundaries as defect sinks under irradiation in LiAlO2 and LiAl5O8

Citation Formats

References (62)

Similar Records

Related Subjects

Molecular dynamics study of grain boundaries as defect sinks under irradiation in LiAlO₂ and LiAl₅O₈