In-situ re-crystallization of heavily-irradiated Gd2Ti2O7
Abstract
Gadolinium titanate (Gd2Ti2O7, or GTO) and other lanthanide pyrochlores are interesting candidates for actinide waste disposal and fast ion conduction because the relevant material properties are intimately dependent on local cation structure. Therefore, a deep understanding of the kinetics associated with cation ordering and disordering is required if such material properties are to be tuned for specific device designs. To this end, single crystals of GTO were irradiated with 190 keV helium ions to a total fluence of 1 × 1017 ions/cm2, amorphizing the sample surface to a depth of ~1 μm and resulting in significant He bubble accumulation. FIB lamellae lifted out from the irradiated sections were examined during heat treatment in the (scanning) transmission electron microscope. Two distinct stages of the re-crystallization of the amorphized material were observed. The material near the end of the ions’ range transformed first and with the same orientation as the pristine material. This was due to the close proximity of the pristine material and the presence of small defect fluorite seeds, but the propagation of this growth front was frustrated by the large pores (formerly bubbles) in the He accumulation layer. This was followed by heterogeneous nucleation of new crystallites at randommore »
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Houston, TX (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC). Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1630875
- Report Number(s):
- LA-UR-19-32263
Journal ID: ISSN 1359-6454
- Grant/Contract Number:
- 89233218CNA000001
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Acta Materialia
- Additional Journal Information:
- Journal Volume: 194; Journal Issue: C; Journal ID: ISSN 1359-6454
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; pyrochlore; ion irradiation; in situ; STEM; crystallization
Citation Formats
Janish, Matthew Thomas, Schneider, Matthew M., Valdez, James Anthony, Mcclellan, Kenneth James, Byler, Darrin David, Wang, Yongqiang, Chen, Di, Holesinger, Terry George, and Uberuaga, Blas P. In-situ re-crystallization of heavily-irradiated Gd2Ti2O7. United States: N. p., 2020.
Web. doi:10.1016/j.actamat.2020.04.026.
Janish, Matthew Thomas, Schneider, Matthew M., Valdez, James Anthony, Mcclellan, Kenneth James, Byler, Darrin David, Wang, Yongqiang, Chen, Di, Holesinger, Terry George, & Uberuaga, Blas P. In-situ re-crystallization of heavily-irradiated Gd2Ti2O7. United States. https://doi.org/10.1016/j.actamat.2020.04.026
Janish, Matthew Thomas, Schneider, Matthew M., Valdez, James Anthony, Mcclellan, Kenneth James, Byler, Darrin David, Wang, Yongqiang, Chen, Di, Holesinger, Terry George, and Uberuaga, Blas P. Thu .
"In-situ re-crystallization of heavily-irradiated Gd2Ti2O7". United States. https://doi.org/10.1016/j.actamat.2020.04.026. https://www.osti.gov/servlets/purl/1630875.
@article{osti_1630875,
title = {In-situ re-crystallization of heavily-irradiated Gd2Ti2O7},
author = {Janish, Matthew Thomas and Schneider, Matthew M. and Valdez, James Anthony and Mcclellan, Kenneth James and Byler, Darrin David and Wang, Yongqiang and Chen, Di and Holesinger, Terry George and Uberuaga, Blas P.},
abstractNote = {Gadolinium titanate (Gd2Ti2O7, or GTO) and other lanthanide pyrochlores are interesting candidates for actinide waste disposal and fast ion conduction because the relevant material properties are intimately dependent on local cation structure. Therefore, a deep understanding of the kinetics associated with cation ordering and disordering is required if such material properties are to be tuned for specific device designs. To this end, single crystals of GTO were irradiated with 190 keV helium ions to a total fluence of 1 × 1017 ions/cm2, amorphizing the sample surface to a depth of ~1 μm and resulting in significant He bubble accumulation. FIB lamellae lifted out from the irradiated sections were examined during heat treatment in the (scanning) transmission electron microscope. Two distinct stages of the re-crystallization of the amorphized material were observed. The material near the end of the ions’ range transformed first and with the same orientation as the pristine material. This was due to the close proximity of the pristine material and the presence of small defect fluorite seeds, but the propagation of this growth front was frustrated by the large pores (formerly bubbles) in the He accumulation layer. This was followed by heterogeneous nucleation of new crystallites at random orientations at the top of the He accumulation layer, which is attributed to the high surface area associated with the many small He bubbles in that region. Finally, it is inferred that the kinetics of grain growth in this material are significantly faster than the kinetics of grain nucleation.},
doi = {10.1016/j.actamat.2020.04.026},
journal = {Acta Materialia},
number = C,
volume = 194,
place = {United States},
year = {Thu May 14 00:00:00 EDT 2020},
month = {Thu May 14 00:00:00 EDT 2020}
}
Web of Science
Works referenced in this record:
Ionic conduction in the Gd2Ti2O7−Gd2Zr2O7 system
journal, September 1988
- Moon, P. K.; Tuller, H. L.
- Solid State Ionics, Vol. 28-30
Oxygen ion conduction and structural disorder in conductive oxides
journal, December 1994
- Tuller, Harry L.
- Journal of Physics and Chemistry of Solids, Vol. 55, Issue 12
Enhanced ionic conductivity in pyrochlore and fluorite mixed phase yttrium-doped lanthanum zirconate
journal, January 2015
- Yang, Fan; Wang, Yanfei; Zhao, Xiaofeng
- Journal of Power Sources, Vol. 273
Structural vs. intrinsic carriers: contrasting effects of cation chemistry and disorder on ionic conductivity in pyrochlores
journal, January 2015
- Perriot, Romain; Uberuaga, Blas P.
- Journal of Materials Chemistry A, Vol. 3, Issue 21
Massively enhanced ionic transport in irradiated crystalline pyrochlore
journal, January 2019
- Kreller, Cortney R.; Valdez, James A.; Holesinger, Terry G.
- Journal of Materials Chemistry A, Vol. 7, Issue 8
Radiation Tolerance of Complex Oxides
journal, August 2000
- Sickafus, K. E.
- Science, Vol. 289, Issue 5480
Radiation-induced amorphization resistance and radiation tolerance in structurally related oxides
journal, February 2007
- Sickafus, Kurt E.; Grimes, Robin W.; Valdez, James A.
- Nature Materials, Vol. 6, Issue 3
Radiation effects in nuclear waste forms for high-level radioactive waste
journal, January 1995
- Ewing, R. C.; Weber, W. J.; Clinard, F. W.
- Progress in Nuclear Energy, Vol. 29, Issue 2
Natural Pyrochlores: Analogues For Actinide Host Phases in Radioactive Waste Forms
journal, January 1984
- Lumpkin, Gregory R.; Ewing, Rodney C.
- MRS Proceedings, Vol. 44
Potential benefit of amorphization in the retention of gaseous species in irradiated pyrochlores
journal, February 2019
- Holesinger, Terry G.; Valdez, James A.; Janish, Matthew T.
- Acta Materialia, Vol. 164
Intricate disorder in defect fluorite/pyrochlore: a concord of chemistry and crystallography
journal, June 2017
- Simeone, David; Thorogood, Gordon James; Huo, Da
- Scientific Reports, Vol. 7, Issue 1
Evidence for percolation diffusion of cations and reordering in disordered pyrochlore from accelerated molecular dynamics
journal, September 2017
- Perriot, Romain; Uberuaga, Blas P.; Zamora, Richard J.
- Nature Communications, Vol. 8, Issue 1
An in situ X ray diffraction study of the kinetics of the Ni 2 SiO 4 olivine-spinel transformation
journal, January 1990
- Rubie, D. C.; Tsuchida, Y.; Yagi, T.
- Journal of Geophysical Research, Vol. 95, Issue B10
Kinetics of the peritectic phase transformation: In-situ measurements and phase field modeling
journal, March 2006
- Phelan, Dominic; Reid, Mark; Dippenaar, Rian
- Metallurgical and Materials Transactions A, Vol. 37, Issue 3
Growth processes and phase transformations studied in situ transmission electron microscopy
journal, July 2000
- Ross, F. M.
- IBM Journal of Research and Development, Vol. 44, Issue 4
Combined effects of radiation damage and He accumulation on bubble nucleation in Gd2Ti2O7
journal, October 2016
- Taylor, Caitlin A.; Patel, Maulik K.; Aguiar, Jeffery A.
- Journal of Nuclear Materials, Vol. 479
Bubble formation and lattice parameter changes resulting from He irradiation of defect-fluorite Gd2Zr2O7
journal, August 2016
- Taylor, Caitlin A.; Patel, Maulik K.; Aguiar, Jeffery A.
- Acta Materialia, Vol. 115
Swift heavy ion track formation in Gd2Zr2−Ti O7 pyrochlore: Effect of electronic energy loss
journal, October 2014
- Lang, Maik; Toulemonde, Marcel; Zhang, Jiaming
- Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 336
Response of Gd2Ti2O7 and La2Ti2O7 to swift-heavy ion irradiation and annealing
journal, July 2015
- Park, Sulgiye; Lang, Maik; Tracy, Cameron L.
- Acta Materialia, Vol. 93
Structural response of titanate pyrochlores to swift heavy ion irradiation
journal, September 2016
- Shamblin, Jacob; Tracy, Cameron L.; Ewing, Rodney C.
- Acta Materialia, Vol. 117
Direct observations of the annealing of prismatic dislocation loops and of climb of dislocations in quenched aluminium
journal, January 1960
- Silcox, J.; Whelan, M. J.
- Philosophical Magazine, Vol. 5, Issue 49
Crystallization kinetics and microstructure-dependent leakage current behavior of ultrathin HfO2 dielectrics: In situ annealing studies
journal, March 2004
- Kim, Hyoungsub; Marshall, Ann; McIntyre, Paul C.
- Applied Physics Letters, Vol. 84, Issue 12
In?Situ Transmission Electron Microscopy Crystallization Studies of Sol?Gel-Derived Barium Titanate Thin Films
journal, November 1997
- Gust, Maria C.; Evans, Neal D.; Momoda, Leslie A.
- Journal of the American Ceramic Society, Vol. 80, Issue 11
In situ TEM imaging of CaCO3 nucleation reveals coexistence of direct and indirect pathways
journal, September 2014
- Nielsen, M. H.; Aloni, S.; De Yoreo, J. J.
- Science, Vol. 345, Issue 6201
In-Situ Tem Studies of Recrystallization and Grain Growth in Al-Mg-Mn-Zr Alloys
journal, January 1995
- Vetrano, John S.; Bruemmer, Steve M.; Robertson, Ian M.
- MRS Proceedings, Vol. 404
Nucleation and growth of Ω phase in Al-4.0 Cu-0.5 Mg-0.5 Ag alloy—An in situ hot-stage TEM study
journal, August 1991
- Garg, A.; Howe, J. M.
- Acta Metallurgica et Materialia, Vol. 39, Issue 8
In situ transmission electron microscopy study of the crystallization of Ge2Sb2Te5
journal, February 2004
- Kooi, B. J.; Groot, W. M. G.; De Hosson, J. Th. M.
- Journal of Applied Physics, Vol. 95, Issue 3
In situ transmission electron microscopy studies of silicide‐mediated crystallization of amorphous silicon
journal, January 1992
- Hayzelden, C.; Batstone, J. L.; Cammarata, R. C.
- Applied Physics Letters, Vol. 60, Issue 2
Mapping Cation Disorder in Irradiated Gd 2 Ti 2 O 7 Pyrochlore by 4D-STEM
journal, August 2019
- Janish, Matthew T.; Schneider, Matthew M.; Ophus, Colin
- Microscopy and Microanalysis, Vol. 25, Issue S2
Behaviour of TEM metal grids during in-situ heating experiments
journal, May 2009
- Zhang, Zaoli; Su, Dangsheng
- Ultramicroscopy, Vol. 109, Issue 6
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011
- Momma, Koichi; Izumi, Fujio
- Journal of Applied Crystallography, Vol. 44, Issue 6
A pyramid approach to subpixel registration based on intensity
journal, January 1998
- Thevenaz, P.; Ruttimann, U. E.; Unser, M.
- IEEE Transactions on Image Processing, Vol. 7, Issue 1
Thermodynamic and structural evolution of Dy2Ti2O7 pyrochlore after swift heavy ion irradiation
journal, February 2018
- Chung, Cheng-Kai; Shamblin, Jacob; O'Quinn, Eric C.
- Acta Materialia, Vol. 145
Ion-induced damage accumulation and electron-beam-enhanced recrystallization in
journal, September 2005
- Zhang, Y.; Lian, J.; Wang, C. M.
- Physical Review B, Vol. 72, Issue 9
Using Machine Learning To Identify Factors That Govern Amorphization of Irradiated Pyrochlores
journal, November 2016
- Pilania, Ghanshyam; Whittle, Karl R.; Jiang, Chao
- Chemistry of Materials, Vol. 29, Issue 6
The development of grain-face porosity in irradiated oxide fuel
journal, February 2004
- White, R. J.
- Journal of Nuclear Materials, Vol. 325, Issue 1