Inferring relative dose-dependent color center populations in proton irradiated thoria single crystals using optical spectroscopy

Khanolkar, Amey Rajendra; Dennett, Cody Andrew; Hua, Zilong; Mann, J. Matthew; Hurley, David H.; Khafizov, Marat

doi:10.1039/d1cp05191a

Title: Inferring relative dose-dependent color center populations in proton irradiated thoria single crystals using optical spectroscopy

Journal Article · 20 February 2022 · Physical Chemistry Chemical Physics. PCCP

DOI: https://doi.org/10.1039/d1cp05191a · OSTI ID:1889705

^[1];

^[1]; Mann, J. Matthew ^[2]; Hurley, David H. ^[1];

^[3]

Idaho National Lab. (INL), Idaho Falls, ID (United States)
Air Force Research Lab. (AFRL), Wright-Patterson AFB, OH (United States)
The Ohio State Univ., Columbus, OH (United States)

In this work, we have utilized photoluminescence spectroscopy and optical ellipsometry to characterize the dose-dependence of the photoluminescence emission intensity and changes in optical absorption of thoria single crystals subject to irradiation with energetic protons at room- and elevated-temperatures. The photoluminescence peaks and the optical absorption bands are attributed to creation of new electronic states emerging from defects resulting from displacement damage. These bands are most likely associated with electrons trapped at the oxygen vacancy sites similar to color centers formed in other irradiated oxides and halides. Our experimental observations are supported by a standard density functional theory calculation of the electronic structure in pristine and oxygen vacancy-bearing thoria crystals. The dose-dependence of the intensity of the photoluminescence peaks is used to parameterize a rate theory model that estimates the concentration of color centers in the irradiated crystals. This parameterization provides optimized migration barrier parameters for oxygen interstitials and vacancies that simultaneously capture the optical response of the crystals irradiated at room- and elevated-temperature. These optical spectroscopy techniques offer a promising pathway to characterize the population of color centers formed at the sites of oxygen anion vacancies, particularly in irradiated nuclear fuels, where atomic-level defects cannot be readily imaged using electron microscopy. When combined with other direct and indirect characterization tools, our approach can provide new insight into defect formation and accumulation in energy materials over single atomic to extended length scales.

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

Sponsoring Organization:: USDOE; USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 1889705

Report Number(s):: INL/JOU-22-66040-Rev000

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 10 Vol. 24; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (75)

Spectroscopic Ellipsometry Fujiwara, Hiroyuki https://doi.org/10.1002/9780470060193	book	January 2007
Positron Annihilation in Semiconductors Krause-Rehberg, Reinhard; Leipner, Hartmut S. Springer Series in Solid-State Sciences https://doi.org/10.1007/978-3-662-03893-2	book	January 1999
�ber Erregung und Entf�rbung lichtelektrisch leitender Alkalihalogenide Smakula, Alexander Zeitschrift f�r Physik, Vol. 59, Issue 9-10 https://doi.org/10.1007/BF01344801	journal	September 1930
The optical absorption spectra of thorium oxide Bodine, J. H.; Thiess, F. B. Journal of the Franklin Institute, Vol. 259, Issue 6 https://doi.org/10.1016/0016-0032(55)90111-3	journal	June 1955
Luminescence of thin uranium oxide films Winer, K.; Wooten, F.; Colmenares, C. A. Journal of Luminescence, Vol. 35, Issue 6 https://doi.org/10.1016/0022-2313(86)90017-7	journal	September 1986
A review of the optical properties of anion lattice vacancies, and electrical conduction in α-Al₂O₃: their relation to radiation-induced electrical degradation Evans, Bruce D. Journal of Nuclear Materials, Vol. 219, p. 202-223 https://doi.org/10.1016/0022-3115(94)00529-X	journal	March 1995
Thermoluminescence and fluorescence in thoria Harvey, P. J.; Hallett, J. B. Journal of Solid State Chemistry, Vol. 12, Issue 3-4 https://doi.org/10.1016/0022-4596(75)90309-6	journal	January 1975
Band gaps, crystal-field splitting, spin-orbit coupling, and exciton binding energies in ZnO under hydrostatic pressure Mang, A.; Reimann, K.; Rübenacke, St. Solid State Communications, Vol. 94, Issue 4 https://doi.org/10.1016/0038-1098(95)00054-2	journal	April 1995
Rutherford backscattering spectrometry Perrière, Jaques Vacuum, Vol. 37, Issue 5-6 https://doi.org/10.1016/0042-207X(87)90327-7	journal	January 1987
Primary Radiation Damage Formation Stoller, R. E. Comprehensive Nuclear Materials https://doi.org/10.1016/B978-0-08-056033-5.00027-6	book	January 2012
Radiation-induced point defects in simple oxides Kotomin, E. A.; Popov, A. I. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 141, Issue 1-4 https://doi.org/10.1016/S0168-583X(98)00079-2	journal	May 1998
Combining mesoscale thermal transport and x-ray diffraction measurements to characterize early-stage evolution of irradiation-induced defects in ceramics Khafizov, Marat; Riyad, M. Faisal; Wang, Yuzhou Acta Materialia, Vol. 193 https://doi.org/10.1016/j.actamat.2020.04.018	journal	July 2020
Phase and defect evolution in uranium-nitrogen-oxygen system under irradiation He, Lingfeng; Khafizov, Marat; Jiang, Chao Acta Materialia, Vol. 208 https://doi.org/10.1016/j.actamat.2021.116778	journal	April 2021
An integrated experimental and computational investigation of defect and microstructural effects on thermal transport in thorium dioxide Dennett, Cody A.; Deskins, W. Ryan; Khafizov, Marat Acta Materialia, Vol. 213 https://doi.org/10.1016/j.actamat.2021.116934	journal	July 2021
Consequences of lead incorporation in fluorite structured thoria Kumar, Manish; Tripathi, Vikash Kumar; Nagarajan, Rajamani Ceramics International, Vol. 45, Issue 9 https://doi.org/10.1016/j.ceramint.2019.03.046	journal	June 2019
Predicting damage production in monoatomic and multi-elemental targets using stopping and range of ions in matter code: Challenges and recommendations Weber, William J.; Zhang, Yanwen Current Opinion in Solid State and Materials Science, Vol. 23, Issue 4 https://doi.org/10.1016/j.cossms.2019.06.001	journal	August 2019
Kr and Xe irradiations in lanthanum (La) doped ceria: Study at the high dose regime Yun, Di; Oaks, Aaron J.; Chen, Wei-ying Journal of Nuclear Materials, Vol. 418, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2011.08.005	journal	November 2011
Determination of high burn-up nuclear fuel elastic properties with acoustic microscopy Laux, D.; Baron, D.; Despaux, G. Journal of Nuclear Materials, Vol. 420, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2011.09.010	journal	January 2012
Thermal conductivity of UO2+x and U4O9−y White, J. T.; Nelson, A. T. Journal of Nuclear Materials, Vol. 443, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.07.063	journal	November 2013
Study of temperature and radiation induced microstructural changes in Xe-implanted UO2 by TEM, STEM, SIMS and positron spectroscopy Djourelov, Nikolay; Marchand, Benoît; Marinov, Hristo Journal of Nuclear Materials, Vol. 443, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.07.066	journal	November 2013
Full characterization of dislocations in ion-irradiated polycrystalline UO2 Onofri, C.; Legros, M.; Léchelle, J. Journal of Nuclear Materials, Vol. 494 https://doi.org/10.1016/j.jnucmat.2017.07.043	journal	October 2017
Cluster dynamics simulation of uranium self-diffusion during irradiation in UO2 Matthews, Christopher; Perriot, Romain; Cooper, Michael W. D. Journal of Nuclear Materials, Vol. 527 https://doi.org/10.1016/j.jnucmat.2019.151787	journal	December 2019
Additional complexity in the Raman spectra of U3O8 Miskowiec, A.; Niedziela, J. L.; Spano, T. L. Journal of Nuclear Materials, Vol. 527 https://doi.org/10.1016/j.jnucmat.2019.151790	journal	December 2019
TEM Characterization of Dislocation Loops in Proton Irradiated Single Crystal ThO2 Bawane, Kaustubh; Liu, Xiang; Yao, Tiankai Journal of Nuclear Materials https://doi.org/10.1016/j.jnucmat.2021.152998	journal	April 2021
Indirect characterization of point defects in proton irradiated ceria Chauhan, Vinay S.; Pakarinen, Janne; Yao, Tiankai Materialia, Vol. 15 https://doi.org/10.1016/j.mtla.2021.101019	journal	March 2021
Radiation damage evolution in ceramics Devanathan, Ram 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.2009.06.020	journal	September 2009
SRIM – The stopping and range of ions in matter (2010) Ziegler, James F.; Ziegler, M. D.; Biersack, J. P. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 268, Issue 11-12 https://doi.org/10.1016/j.nimb.2010.02.091	journal	June 2010
Rutherford backscattering and nuclear reaction analyses of hydrogen ion-implanted ZnO bulk single crystals Kaida, T.; Kamioka, K.; Ida, T. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 332 https://doi.org/10.1016/j.nimb.2014.02.020	journal	August 2014
Charged defects during alpha-irradiation of actinide oxides as revealed by Raman and luminescence spectroscopy Mohun, R.; Desgranges, L.; Léchelle, J. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 374 https://doi.org/10.1016/j.nimb.2015.08.003	journal	May 2016
Evolution of extended defects in polycrystalline UO2 under heavy ion irradiation: combined TEM, XRD and Raman study Onofri, C.; Sabathier, C.; Palancher, H. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 374 https://doi.org/10.1016/j.nimb.2015.08.091	journal	May 2016
Effect of ballistic damage in UO2 samples under ion beam irradiations studied by in situ Raman spectroscopy Gutierrez, G.; Onofri, C.; Miro, S. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 434 https://doi.org/10.1016/j.nimb.2018.08.010	journal	November 2018
Thermal transport and optical spectroscopy in 710-MeV Bi ion irradiated LiF crystals Koshkinbayeva, A.; Abdullaev, A.; Nurekeyev, Z. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 475 https://doi.org/10.1016/j.nimb.2020.04.006	journal	July 2020
Role of defects in tailoring structural, electrical and optical properties of ZnO Dutta, Sreetama; Chattopadhyay, S.; Sarkar, A. Progress in Materials Science, Vol. 54, Issue 1 https://doi.org/10.1016/j.pmatsci.2008.07.002	journal	January 2009
Three-dimensional imaging of individual point defects using selective detection angles in annular dark field scanning transmission electron microscopy Johnson, Jared M.; Im, Soohyun; Windl, Wolfgang Ultramicroscopy, Vol. 172 https://doi.org/10.1016/j.ultramic.2016.10.007	journal	January 2017
Thermal Energy Transport in Oxide Nuclear Fuel Hurley, David H.; El-Azab, Anter; Bryan, Matthew S. Chemical Reviews, Vol. 122, Issue 3 https://doi.org/10.1021/acs.chemrev.1c00262	journal	December 2021
Fundamentals and Catalytic Applications of CeO ₂ -Based Materials Montini, Tiziano; Melchionna, Michele; Monai, Matteo Chemical Reviews, Vol. 116, Issue 10 https://doi.org/10.1021/acs.chemrev.5b00603	journal	April 2016
Hydrothermal Growth and Thermal Property Characterization of ThO ₂ Single Crystals Mann, Matthew; Thompson, Daniel; Serivalsatit, Karn Crystal Growth & Design, Vol. 10, Issue 5 https://doi.org/10.1021/cg901308f	journal	May 2010
A Spectroscopic Characterization of the Reduction of Ceria from Electronic Transitions of Intrinsic Point Defects Binet, Claude; Badri, Ahmed; Lavalley, Jean-Claude The Journal of Physical Chemistry, Vol. 98, Issue 25 https://doi.org/10.1021/j100076a025	journal	June 1994
Oxygen Vacancy Formation and Migration in Ce _x Th _{1– x} O ₂ Solid Solution Xiao, H. Y.; Weber, W. J. The Journal of Physical Chemistry B, Vol. 115, Issue 20 https://doi.org/10.1021/jp202016s	journal	May 2011
Ultrastructural Characterization of the Lower Motor System in a Mouse Model of Krabbe Disease Cappello, Valentina; Marchetti, Laura; Parlanti, Paola Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/s41598-016-0001-8	journal	December 2016
Nonlinear propagating modes beyond the phonons in fluorite-structured crystals Bryan, Matthew S.; Fu, Lyuwen; Rickert, Karl Communications Physics, Vol. 3, Issue 1 https://doi.org/10.1038/s42005-020-00483-2	journal	November 2020
Metal oxide-based materials as an emerging family of hydrogen evolution electrocatalysts Zhu, Yinlong; Lin, Qian; Zhong, Yijun Energy & Environmental Science, Vol. 13, Issue 10 https://doi.org/10.1039/D0EE02485F	journal	January 2020
Optical absorption spectroscopy of thorium dioxide. Analysis of oxidising and reducing anneals and gamma and UV radiation on both flux-grown and arc-fused single crystals Griffiths, Trevor R.; Dixon, James Journal of the Chemical Society, Faraday Transactions, Vol. 88, Issue 8 https://doi.org/10.1039/ft9928801149	journal	January 1992
Optical performance of nanocrystalline transparent ceria films Patsalas, P.; Logothetidis, S.; Metaxa, C. Applied Physics Letters, Vol. 81, Issue 3 https://doi.org/10.1063/1.1494458	journal	July 2002
Optical absorption and luminescence energies of F centers in CaO from ab initio embedded cluster calculations Carrasco, Javier; Sousa, Carmen; Illas, Francesc The Journal of Chemical Physics, Vol. 125, Issue 7 https://doi.org/10.1063/1.2337292	journal	August 2006
Identification of sub-band-gap absorption features at the HfO2∕Si(100) interface via spectroscopic ellipsometry Price, J.; Lysaght, P. S.; Song, S. C. Applied Physics Letters, Vol. 91, Issue 6 https://doi.org/10.1063/1.2769389	journal	August 2007
Optical waveguides in lithium niobate: Recent developments and applications Bazzan, Marco; Sada, Cinzia Applied Physics Reviews, Vol. 2, Issue 4 https://doi.org/10.1063/1.4931601	journal	December 2015
Review and perspective: Sapphire optical fiber cladding development for harsh environment sensing Chen, Hui; Buric, Michael; Ohodnicki, Paul R. Applied Physics Reviews, Vol. 5, Issue 1 https://doi.org/10.1063/1.5010184	journal	March 2018
Band-to-band transitions and critical points in the near-infrared to vacuum ultraviolet dielectric functions of single crystal urania and thoria Mock, Alyssa; Dugan, Christina; Knight, Sean Applied Physics Letters, Vol. 114, Issue 21 https://doi.org/10.1063/1.5087059	journal	May 2019
Vacancy defects induced changes in the electronic and optical properties of NiO studied by spectroscopic ellipsometry and first-principles calculations Egbo, Kingsley O.; Liu, Chao Ping; Ekuma, Chinedu E. Journal of Applied Physics, Vol. 128, Issue 13 https://doi.org/10.1063/5.0021650	journal	October 2020
The influence of lattice defects, recombination, and clustering on thermal transport in single crystal thorium dioxide Dennett, Cody A.; Hua, Zilong; Khanolkar, Amey APL Materials, Vol. 8, Issue 11 https://doi.org/10.1063/5.0025384	journal	November 2020
Photoluminescence properties of additively coloured MgO. I. Effects of uniaxial stress and ODMR Edel, P.; d'Aubigne, Y. M.; Romestain, R. Journal of Physics C: Solid State Physics, Vol. 12, Issue 23 https://doi.org/10.1088/0022-3719/12/23/028	journal	December 1979
F Centers in Thorium Oxide Neeley, V. I.; Gruber, J. B.; Gray, W. J. Physical Review, Vol. 158, Issue 3 https://doi.org/10.1103/PhysRev.158.809	journal	June 1967
Luminescence of the F + Center in MgO Chen, Y.; Kolopus, J. L.; Sibley, W. A. Physical Review, Vol. 186, Issue 3 https://doi.org/10.1103/PhysRev.186.865	journal	October 1969
Optical Properties of Crystalline Thoria Weinreich, O. A.; Danforth, W. E. Physical Review, Vol. 88, Issue 4 https://doi.org/10.1103/PhysRev.88.953.2	journal	November 1952
Molecular Dynamics Simulation of Thermal Transport in UO 2 Containing Uranium, Oxygen, and Fission-product Defects Liu, X. -Y.; Cooper, M. W. D.; McClellan, K. J. Physical Review Applied, Vol. 6, Issue 4 https://doi.org/10.1103/PhysRevApplied.6.044015	journal	October 2016
F + and F ′ Centers in Magnesium Oxide Kappers, Lawrence A.; Kroes, Roger L.; Hensley, Eugene B. Physical Review B, Vol. 1, Issue 10 https://doi.org/10.1103/PhysRevB.1.4151	journal	May 1970
Self-interaction correction to density-functional approximations for many-electron systems Perdew, J. P.; Zunger, Alex Physical Review B, Vol. 23, Issue 10, p. 5048-5079 https://doi.org/10.1103/PhysRevB.23.5048	journal	May 1981
Electronic Defect Structure of Single-Crystal Th O 2 by Thermoluminescence Rodine, Elward T.; Land, Peter L. Physical Review B, Vol. 4, Issue 8 https://doi.org/10.1103/PhysRevB.4.2701	journal	October 1971
Color-center creation in LiF under irradiation with swift heavy ions: Dependence on energy loss and fluence Schwartz, K.; Trautmann, C.; El-Said, A. S. Physical Review B, Vol. 70, Issue 18 https://doi.org/10.1103/PhysRevB.70.184104	journal	November 2004
Positron annihilation lifetime spectroscopy of ZnO bulk samples Zubiaga, A.; Plazaola, F.; García, J. A. Physical Review B, Vol. 76, Issue 8 https://doi.org/10.1103/PhysRevB.76.085202	journal	August 2007
Optical excitation of deep defect levels in insulators within many-body perturbation theory: The F center in calcium fluoride Ma, Yuchen; Rohlfing, Michael Physical Review B, Vol. 77, Issue 11 https://doi.org/10.1103/PhysRevB.77.115118	journal	March 2008
Mechanical and electronic properties of CeO 2 , ThO 2 , and ( Ce , Th ) O 2 alloys Sevik, C.; Çağın, T. Physical Review B, Vol. 80, Issue 1 https://doi.org/10.1103/PhysRevB.80.014108	journal	July 2009
F center in lithium fluoride revisited: Comparison of solid-state physics and quantum-chemistry approaches Karsai, Ferenc; Tiwald, Paul; Laskowski, Robert Physical Review B, Vol. 89, Issue 12 https://doi.org/10.1103/PhysRevB.89.125429	journal	March 2014
Ab initio perspective on the Mollwo-Ivey relation for F centers in alkali halides Tiwald, Paul; Karsai, Ferenc; Laskowski, Robert Physical Review B, Vol. 92, Issue 14 https://doi.org/10.1103/PhysRevB.92.144107	journal	October 2015
First-Principles Optical Spectra for F Centers in MgO Rinke, Patrick; Schleife, André; Kioupakis, Emmanouil Physical Review Letters, Vol. 108, Issue 12 https://doi.org/10.1103/PhysRevLett.108.126404	journal	March 2012
Lattice strain in irradiated materials unveils a prevalent defect evolution mechanism Debelle, Aurélien; Crocombette, Jean-Paul; Boulle, Alexandre Physical Review Materials, Vol. 2, Issue 1 https://doi.org/10.1103/PhysRevMaterials.2.013604	journal	January 2018
In situ defect annealing of swift heavy ion irradiated CeO ₂ and ThO ₂ using synchrotron X-ray diffraction and a hydrothermal diamond anvil cell Palomares, Raul I.; Tracy, Cameron L.; Zhang, Fuxiang Journal of Applied Crystallography, Vol. 48, Issue 3 https://doi.org/10.1107/S160057671500477X	journal	April 2015
Color Centers and Point Defects in Irradiated Thoria Childs, B. G.; Harvey, P. J.; Hallett, J. B. Journal of the American Ceramic Society, Vol. 53, Issue 8 https://doi.org/10.1111/j.1151-2916.1970.tb12671.x	journal	August 1970
Optical Absorption Spectroscopy of ThO ₂ Childs, B. G.; Harvey, P. J.; Hallett, J. B. Journal of the American Ceramic Society, Vol. 55, Issue 11 https://doi.org/10.1111/j.1151-2916.1972.tb13433.x	journal	November 1972
Effects of He Irradiation on Yttria-Stabilized Zirconia Ceramics Yang, Tengfei; Taylor, Caitlin A.; Wang, Chenxu Journal of the American Ceramic Society, Vol. 98, Issue 4 https://doi.org/10.1111/jace.13423	journal	December 2014
Impact of irradiation induced dislocation loops on thermal conductivity in ceramics Khafizov, Marat; Pakarinen, Janne; He, Lingfeng Journal of the American Ceramic Society, Vol. 102, Issue 12 https://doi.org/10.1111/jace.16616	journal	June 2019
Factors Influencing the Photoluminescence Behavior of Thoria Harvey, P. J.; Hallett, J. B. Journal of The Electrochemical Society, Vol. 123, Issue 3 https://doi.org/10.1149/1.2132835	journal	March 1976
Transmission and reflection ellipsometry of thin films and multilayer systems Bader, G.; Ashrit, P. V.; Truong, Vo-Van Applied Optics, Vol. 37, Issue 7 https://doi.org/10.1364/AO.37.001146	journal	January 1998
A review on cerium oxide-based electrolytes for ITSOFC Arunkumar, P.; Meena, M.; Babu, K. Suresh Nanomaterials and Energy, Vol. 1, Issue 5 https://doi.org/10.1680/nme.12.00015	journal	September 2012

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Title: Inferring relative dose-dependent color center populations in proton irradiated thoria single crystals using optical spectroscopy

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