Bulk and Short-Circuit Anion Diffusion in Epitaxial Fe2O3 Films Quantified Using Buried Isotopic Tracer Layers

Kaspar, Tiffany C.; Taylor, Sandra D.; Yano, Kayla H.; Lach, Timothy G.; Zhou, Yadong; Zhu, Zihua; Kohnert, Aaron Anthony; Still, Evan K.; Hosemann, Peter; Spurgeon, Steven R.; Schreiber, Daniel K.

doi:10.1002/admi.202001768

Title: Bulk and Short-Circuit Anion Diffusion in Epitaxial Fe₂O₃ Films Quantified Using Buried Isotopic Tracer Layers

Journal Article · Tue Mar 09 00:00:00 EST 2021 · Advanced Materials Interfaces

DOI:https://doi.org/10.1002/admi.202001768· OSTI ID:1783601

^[1]; Taylor, Sandra D. ^[1]; Yano, Kayla H. ^[1];

^[1]; Zhou, Yadong ^[1];

^[1]; Kohnert, Aaron Anthony ^[2]; Still, Evan K. ^[3]; Hosemann, Peter ^[3];

^[1]; Schreiber, Daniel K. ^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of California, Berkeley, CA (United States)

Self-diffusion is a fundamental physical process that, in solid materials, is intimately correlated with both microstructure and functional properties. In this work, a universal approach is presented to precisely characterize self-diffusion in ionic solids by isotopically enriching anions and/or cations at specific locations within an epitaxial film stack, and characterize their redistribution at high spatial resolution with atom probe tomography. Nanoscale anion diffusivity is quantified in epitaxial α-Fe₂O₃ thin films deposited by molecular beam epitaxy with a thin (10 nm) buried layer highly enriched in ¹⁸O. The isotopic sensitivity of the atom probe allows precise measurement of ¹⁸O distribution across the sharp interfaces between this layer and the surrounding Fe₂O₃ after annealing. Short-circuit anion diffusion through 1D and 2D structural defects in Fe₂O₃ are also directly visualized in 3D. This versatile approach to study precisely tailored thin film samples at high spatial and mass fidelity will facilitate a deeper understanding of atomic-scale diffusion phenomena.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC05-76RL01830; 89233218CNA000001

OSTI ID:: 1783601

Alternate ID(s):: OSTI ID: 1804202; OSTI ID: 1808842

Report Number(s):: PNNL-SA-155914; LA-UR-21-20331

Journal Information:: Advanced Materials Interfaces, Vol. 8, Issue 9; ISSN 2196-7350

Publisher:: Wiley-VCHCopyright Statement

Country of Publication:: United States

Language:: English

References (65)

Assessment of nitrogen incorporation in dilute GaAsN films using isotopically enriched molecular beam epitaxy and resonant nuclear reaction analysis Demaree, John D.; Svensson, Stefan P.; Sarney, Wendy L. Journal of Vacuum Science & Technology B, Nanotechnology and Microelectronics: Materials, Processing, Measurement, and Phenomena, Vol. 35, Issue 2 https://doi.org/10.1116/1.4977022	journal	March 2017
Oxidation-enhanced Si self-diffusion in isotopically modulated silicon nanopillars Kiga, Ryotaro; Hayashi, Sayaka; Miyamoto, Satoru Journal of Applied Physics, Vol. 127, Issue 4 https://doi.org/10.1063/1.5134105	journal	January 2020
Issues and challenges facing rechargeable lithium batteries Tarascon, J.-M.; Armand, M. Nature, Vol. 414, Issue 6861, p. 359-367 https://doi.org/10.1038/35104644	journal	November 2001
Quantitative assessment of intergranular damage due to PWR primary water exposure in structural Ni-based alloys Ter-Ovanessian, Benoît; Deleume, Julien; Cloué, Jean-Marc Corrosion Science, Vol. 67 https://doi.org/10.1016/j.corsci.2012.09.048	journal	February 2013
Grain boundary diffusion of chromium in polycrystalline nickel studied by SIMS Gheno, Thomas; Jomard, François; Desgranges, Clara Materialia, Vol. 6 https://doi.org/10.1016/j.mtla.2019.100283	journal	June 2019
Oxygen Surface Exchange and Tracer Diffusion in Differently Oriented Thin Films of Gd-Doped CeO ₂ Waldow, Stephan P.; Statham, Benjamin J.; Wardenga, Hans F. ACS Applied Materials & Interfaces, Vol. 12, Issue 32 https://doi.org/10.1021/acsami.0c09605	journal	July 2020
Comparative depth-profiling analysis of nanometer-metal multilayers by ion-probing techniques Escobar Galindo, R.; Gago, R.; Albella, J. M. TrAC Trends in Analytical Chemistry, Vol. 28, Issue 4 https://doi.org/10.1016/j.trac.2009.01.004	journal	April 2009
Controlling Oxygen Mobility in Ruddlesden–Popper Oxides Lee, Dongkyu; Lee, Ho Materials, Vol. 10, Issue 4 https://doi.org/10.3390/ma10040368	journal	March 2017
Microstructure design for fast oxygen conduction Aidhy, Dilpuneet S.; Weber, William J. Journal of Materials Research, Vol. 31, Issue 1 https://doi.org/10.1557/jmr.2015.327	journal	November 2015
Nano- and micro-geochronology in Hadean and Archean zircons by atom-probe tomography and SIMS: New tools for old minerals Valley, John W.; Reinhard, David A.; Cavosie, Aaron J. American Mineralogist, Vol. 100, Issue 7 https://doi.org/10.2138/am-2015-5134	journal	July 2015
Atom probe study of impurity segregation at grain boundaries in chromia scales grown in CO2 gas Nguyen, Thuan Dinh; La Fontaine, Alexandre; Yang, Limei Corrosion Science, Vol. 132 https://doi.org/10.1016/j.corsci.2017.12.024	journal	March 2018
Self-diffusion in α-Fe2O3 natural single crystals Amami, B.; Addou, M.; Millot, F. Ionics, Vol. 5, Issue 5-6 https://doi.org/10.1007/BF02376000	journal	September 1999
Synthesis of epitaxial films of Fe3O4 and α-Fe2O3 with various low-index orientations by oxygen-plasma-assisted molecular beam epitaxy Gao, Y.; Kim, Y. J.; Chambers, S. A. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 15, Issue 2 https://doi.org/10.1116/1.580488	journal	March 1997
Oxygen self-diffusion studies using negative-ion secondary ion mass spectrometry (SIMS) Kilner, J.; Steele, B.; Ilkov, L. Solid State Ionics, Vol. 12 https://doi.org/10.1016/0167-2738(84)90134-6	journal	March 1984
Porous anodic alumina: fabrication, characterization and applications Thompson, G. E. Thin Solid Films, Vol. 297, Issue 1-2 https://doi.org/10.1016/S0040-6090(96)09440-0	journal	April 1997
Growth and characterization of 28Sin/30Sin isotope superlattices Kojima, T.; Nebashi, R.; Itoh, K. M. Applied Physics Letters, Vol. 83, Issue 12 https://doi.org/10.1063/1.1613365	journal	September 2003
Nanoscale resetting of the Th/Pb system in an isotopically-closed monazite grain: A combined atom probe and transmission electron microscopy study Seydoux-Guillaume, A. -M.; Fougerouse, D.; Laurent, A. T. Geoscience Frontiers, Vol. 10, Issue 1 https://doi.org/10.1016/j.gsf.2018.09.004	journal	January 2019
Progress in material selection for solid oxide fuel cell technology: A review Mahato, Neelima; Banerjee, Amitava; Gupta, Alka Progress in Materials Science, Vol. 72 https://doi.org/10.1016/j.pmatsci.2015.01.001	journal	July 2015
The formation of aluminum oxide scales on high-temperature alloys Prescott, R.; Graham, M. J. Oxidation of Metals, Vol. 38, Issue 3-4 https://doi.org/10.1007/BF00666913	journal	October 1992
Three-Dimensional Atom-Probe Tomography: Advances and Applications Seidman, David N. Annual Review of Materials Research, Vol. 37, Issue 1 https://doi.org/10.1146/annurev.matsci.37.052506.084200	journal	August 2007
In situ lift-out: Steps to improve yield and a comparison with other FIB TEM sample preparation techniques Langford, R. M.; Rogers, M. Micron, Vol. 39, Issue 8 https://doi.org/10.1016/j.micron.2008.02.006	journal	December 2008
Self-diffusion in germanium isotope multilayers at low temperatures Hüger, E.; Tietze, U.; Lott, D. Applied Physics Letters, Vol. 93, Issue 16 https://doi.org/10.1063/1.3002294	journal	October 2008
Creation and Ordering of Oxygen Vacancies at WO 3−δ and Perovskite Interfaces Zhang, Kelvin H. L.; Li, Guoqiang; Spurgeon, Steven R. ACS Applied Materials & Interfaces, Vol. 10, Issue 20 https://doi.org/10.1021/acsami.8b03278	journal	April 2018
Oxygen diffusion in nanocrystalline yttria-stabilized zirconia: the effect of grain boundaries De Souza, Roger A.; Pietrowski, Martha J.; Anselmi-Tamburini, Umberto Physical Chemistry Chemical Physics, Vol. 10, Issue 15 https://doi.org/10.1039/b719363g	journal	January 2008
Diffusion of Cation Impurities through Ceria Grain Boundaries Kwak, No Woo; Lim, Dae‐Kwang; Jeong, Seung Jin Advanced Materials Interfaces, Vol. 7, Issue 20 https://doi.org/10.1002/admi.202000688	journal	August 2020
Oxygen transport in La1−xSrxMn1−yCoyO3±δ perovskites De Souza, R. A.; Kilner, J. A. Solid State Ionics, Vol. 126, Issue 1-2 https://doi.org/10.1016/S0167-2738(99)00228-3	journal	November 1999
Correlative Atom Probe Tomography and Transmission Electron Microscopy Analysis of Grain Boundaries in Thermally Grown Alumina Scale Povstugar, Ivan; Weber, Juliane; Naumenko, Dmitry Microscopy and Microanalysis, Vol. 25, Issue 1 https://doi.org/10.1017/S143192761801557X	journal	February 2019
Ceramic Fuel Cells Minh, Nguyen Q. Journal of the American Ceramic Society, Vol. 76, Issue 3 https://doi.org/10.1111/j.1151-2916.1993.tb03645.x	journal	March 1993
Primary radiation damage: A review of current understanding and models Nordlund, Kai; Zinkle, Steven J.; Sand, Andrea E. Journal of Nuclear Materials, Vol. 512 https://doi.org/10.1016/j.jnucmat.2018.10.027	journal	December 2018
Radiation-induced solute segregation in metallic alloys Ardell, Alan J.; Bellon, Pascal Current Opinion in Solid State and Materials Science, Vol. 20, Issue 3 https://doi.org/10.1016/j.cossms.2015.11.001	journal	June 2016
Oxygen transport in La1−xSrxMn1−yCoyO3±δ perovskites Part I. Oxygen tracer diffusion De Souza, R. Solid State Ionics, Vol. 106, Issue 3-4 https://doi.org/10.1016/S0167-2738(97)00499-2	journal	February 1998
A novel approach to determine the local burnup in irradiated fuels using Atom Probe Tomography (APT) Bachhav, Mukesh; Gan, Jian; Keiser, Dennis Journal of Nuclear Materials, Vol. 528 https://doi.org/10.1016/j.jnucmat.2019.151853	journal	January 2020
Impact of lattice mismatch and stoichiometry on the structure and bandgap of (Fe,Cr) ₂ O ₃ epitaxial thin films Kaspar, T. C.; Chamberlin, S. E.; Bowden, M. E. Journal of Physics: Condensed Matter, Vol. 26, Issue 13 https://doi.org/10.1088/0953-8984/26/13/135005	journal	March 2014
A comparative review of the aqueous corrosion of glasses, crystalline ceramics, and metals Frankel, Gerald S.; Vienna, John D.; Lian, Jie npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-018-0037-2	journal	May 2018
Quantitative comparison of sink efficiency of Cu–Nb, Cu–V and Cu–Ni interfaces for point defects Mao, Shimin; Shu, Shipeng; Zhou, Jian Acta Materialia, Vol. 82 https://doi.org/10.1016/j.actamat.2014.09.011	journal	January 2015
Neutron Reflectometry: A Tool to Investigate Diffusion Processes in Solids on the Nanometer Scale Schmidt, Harald; Hüger, Erwin; Chakravarty, Sujoy Advanced Engineering Materials, Vol. 11, Issue 6 https://doi.org/10.1002/adem.200800325	journal	June 2009
A compact, ultra-high vacuum ion source for isotopically enriching and depositing ²⁸ Si thin films Tang, K.; Kim, H. S.; Ramanayaka, A. N. R. Review of Scientific Instruments, Vol. 90, Issue 8 https://doi.org/10.1063/1.5097937	journal	August 2019
Diffusion in energy materials: Governing dynamics from atomistic modelling Parfitt, D.; Kordatos, A.; Filippatos, P. P. Applied Physics Reviews, Vol. 4, Issue 3 https://doi.org/10.1063/1.5001276	journal	September 2017
Experimental observations in support of the dynamic-segregation theory to explain the reactive-element effect Pint, B. A. Oxidation of Metals, Vol. 45, Issue 1-2 https://doi.org/10.1007/BF01046818	journal	February 1996
Visualizing the iron atom exchange front in the Fe(II)-catalyzed recrystallization of goethite by atom probe tomography Taylor, Sandra D.; Liu, Jia; Zhang, Xin Proceedings of the National Academy of Sciences, Vol. 116, Issue 8 https://doi.org/10.1073/pnas.1816620116	journal	February 2019
Analysis of Three-dimensional Atom-probe Data by the Proximity Histogram Hellman, Olof C.; Vandenbroucke, Justin A.; Rüsing, Järg Microscopy and Microanalysis, Vol. 6, Issue 05 https://doi.org/10.1007/S100050010051	journal	September 2000
Oxygen diffusion and surface exchange in the mixed conducting oxides SrTi _1−y Fe _y O _3−δ Metlenko, Veronika; Jung, WooChul; Bishop, Sean R. Physical Chemistry Chemical Physics, Vol. 18, Issue 42 https://doi.org/10.1039/C6CP05756J	journal	January 2016
Iron self-diffusion in Fe ₅ Ge ₃ thin film Merkel, D. G.; Lengyel, A.; Hegedűs, G. Materials Research Express, Vol. 6, Issue 8 https://doi.org/10.1088/2053-1591/ab1c84	journal	May 2019
Bulk and grain boundary Li-diffusion in dense LiMn ₂ O ₄ pellets by means of isotope exchange and ToF-SIMS analysis Schwab, C.; Höweling, A.; Windmüller, A. Physical Chemistry Chemical Physics, Vol. 21, Issue 47 https://doi.org/10.1039/C9CP05128G	journal	January 2019
Electrochemical Energy Storage for Green Grid Yang, Zhenguo; Zhang, Jianlu; Kintner-Meyer, Michael C. W. Chemical Reviews, Vol. 111, Issue 5, p. 3577-3613 https://doi.org/10.1021/cr100290v	journal	May 2011
Oxygen Mobility in Polycrystalline NiCr2O4 and alpha-Fe2O3 Kingery, W. D.; Hill, D. C.; Nelson, R. P. Journal of the American Ceramic Society, Vol. 43, Issue 9 https://doi.org/10.1111/j.1151-2916.1960.tb13699.x	journal	September 1960
Iron oxide surfaces Parkinson, Gareth S. Surface Science Reports, Vol. 71, Issue 1 https://doi.org/10.1016/j.surfrep.2016.02.001	journal	March 2016
Oxygen diffusion in amorphous and partially crystalline gallium oxide von der Heiden, Alexandra; Bornhöfft, Manuel; Mayer, Joachim Physical Chemistry Chemical Physics, Vol. 21, Issue 8 https://doi.org/10.1039/C8CP06439C	journal	January 2019
Investigation of O-18 enriched hematite (α-Fe2O3) by laser assisted atom probe tomography Bachhav, Mukesh; Danoix, Frédéric; Hannoyer, Béatrice International Journal of Mass Spectrometry, Vol. 335 https://doi.org/10.1016/j.ijms.2012.10.012	journal	February 2013
Defect Chemistry: Composition, Transport, and Reactions in the Solid State; Part II: Kinetics Maier, Joachim Angewandte Chemie International Edition in English, Vol. 32, Issue 4 https://doi.org/10.1002/anie.199305281	journal	April 1993
Dynamic Lattice Oxygen Participation on Perovskite LaNiO ₃ during Oxygen Evolution Reaction Liu, Jishan; Jia, Endong; Stoerzinger, Kelsey A. The Journal of Physical Chemistry C, Vol. 124, Issue 28 https://doi.org/10.1021/acs.jpcc.0c04808	journal	June 2020
In situ site-specific specimen preparation for atom probe tomography Thompson, K.; Lawrence, D.; Larson, D. J. Ultramicroscopy, Vol. 107, Issue 2-3 https://doi.org/10.1016/j.ultramic.2006.06.008	journal	February 2007
Atomic-scale age resolution of planetary events White, L. F.; Darling, J. R.; Moser, D. E. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15597	journal	May 2017
Investigation of wüstite (Fe1−xO) by femtosecond laser assisted atom probe tomography Bachhav, M.; Danoix, R.; Danoix, F. Ultramicroscopy, Vol. 111, Issue 6 https://doi.org/10.1016/j.ultramic.2010.11.023	journal	May 2011
Self-diffusion in single crystalline silicon nanowires Südkamp, T.; Hamdana, G.; Descoins, M. Journal of Applied Physics, Vol. 123, Issue 16 https://doi.org/10.1063/1.4996987	journal	April 2018
On the existence and origin of sluggish diffusion in chemically disordered concentrated alloys Osetsky, Yuri N.; Béland, Laurent K.; Barashev, Alexander V. Current Opinion in Solid State and Materials Science, Vol. 22, Issue 3 https://doi.org/10.1016/j.cossms.2018.05.003	journal	June 2018
Smart Align—a new tool for robust non-rigid registration of scanning microscope data Jones, Lewys; Yang, Hao; Pennycook, Timothy J. Advanced Structural and Chemical Imaging, Vol. 1, Issue 1 https://doi.org/10.1186/s40679-015-0008-4	journal	July 2015
Ion-Beam-Induced Atomic Mixing in Ge, Si, and SiGe, Studied by Means of Isotope Multilayer Structures Radek, Manuel; Liedke, Bartosz; Schmidt, Bernd Materials, Vol. 10, Issue 7 https://doi.org/10.3390/ma10070813	journal	July 2017
In situ transmission electron microscopy and spectroscopy studies of rechargeable batteries under dynamic operating conditions: A retrospective and perspective view Wang, Chong-Min Journal of Materials Research, Vol. 30, Issue 3 https://doi.org/10.1557/jmr.2014.281	journal	October 2014
Oxygen Diffusion in MgO and alpha-Fe2O3 Reddy, K. P. R.; Cooper, A. R. Journal of the American Ceramic Society, Vol. 66, Issue 9 https://doi.org/10.1111/j.1151-2916.1983.tb10618.x	journal	September 1983
High-entropy ceramics Oses, Corey; Toher, Cormac; Curtarolo, Stefano Nature Reviews Materials, Vol. 5, Issue 4 https://doi.org/10.1038/s41578-019-0170-8	journal	February 2020
Diffusion and ionic conduction in nanocrystalline ceramics Heitjans, Paul; Indris, Sylvio Journal of Physics: Condensed Matter, Vol. 15, Issue 30 https://doi.org/10.1088/0953-8984/15/30/202	journal	July 2003
Iron self-diffusion in amorphous $Fe Zr ∕ {}^{57}{Fe} Zr$ multilayers measured by neutron reflectometry Gupta, Mukul; Gupta, Ajay; Stahn, J. Physical Review B, Vol. 70, Issue 18 https://doi.org/10.1103/PhysRevB.70.184206	journal	November 2004
Resistive switching materials for information processing Wang, Zhongrui; Wu, Huaqiang; Burr, Geoffrey W. Nature Reviews Materials, Vol. 5, Issue 3 https://doi.org/10.1038/s41578-019-0159-3	journal	January 2020
Effect of analysis direction on the measurement of interfacial mixing in thin metal layers with atom probe tomography Larson, D. J.; Prosa, T. J.; Geiser, B. P. Ultramicroscopy, Vol. 111, Issue 6 https://doi.org/10.1016/j.ultramic.2010.12.010	journal	May 2011

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Title: Bulk and Short-Circuit Anion Diffusion in Epitaxial Fe₂O₃ Films Quantified Using Buried Isotopic Tracer Layers