Directly resolving surface vs. lattice self-diffusion in iron at the nanoscale using in situ atom probe capabilities

Taylor, Sandra D.; Kohnert, Aaron Anthony; Lambeets, Sten V.; Yano, Kayla H.; Still, Evan K.; Simonnin, Pauline G.; Hosemann, Peter; Uberuaga, Blas P.; Kaspar, Tiffany C.; Schreiber, Daniel K.

doi:10.1016/j.mtla.2024.102078

Directly resolving surface vs. lattice self-diffusion in iron at the nanoscale using in situ atom probe capabilities

Journal Article · Thu Apr 04 00:00:00 EDT 2024 · Materialia

DOI:https://doi.org/10.1016/j.mtla.2024.102078· OSTI ID:2432322

^[1]; ^[2]; Lambeets, Sten V. ^[1]; ^[1]; Still, Evan K. ^[3]; ^[1]; ^[3]; ^[2]; ^[1]; Schreiber, Daniel K. ^[1]

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

Surface self-diffusion studies on metals under elevated reaction conditions are limited, as it is inherently challenging to unambiguously follow atomic transport across highly-reactive surfaces. Here, quantitative and mechanistic insight into thermally induced atomic transport processes in bcc α-iron at the sub-nanometer level was achieved using isotopic tracer techniques coupled with in situ atom probe tomography (APT) capabilities. Specifically, using a reactor directly connected to the APT, needle-shaped specimens fabricated from epitaxial thin films with an embedded ⁵⁷Fe tracer layer were annealed in Ar at 500 °C and 350 °C for 1 hour. Furthermore, the tracer was positioned at various depths in the APT specimen by field evaporation, enabling targeted and simultaneous analysis of lattice and surface diffusion. ⁵⁷Fe concentration profiles reveal lattice self-diffusion occurs at 500 °C on the order of ~7 – 9 monolayers, while lattice diffusion is not resolvable at 350 °C. Considerable surface transport was, however, observed at both conditions, where atomic transport over the specimen surface led to the formation of a thin (≤1 nm), isotopically-intermixed layer at the surface. Further, the observed isotopic redistributions at 500 °C were convoluted by additional processes occurring in the subsurface, such as atomic intermixing in correlation with lattice diffusion. However, surface diffusion was determined to be the primary transport process at 350 °C and was thereby quantified. Ultimately, these results demonstrate the significance of surface self-diffusion as a short circuit pathway. More broadly, this approach has the potential to provide detailed insight into (self-)diffusion mechanisms across various materials while targeting site-specific reactions under elevated reaction conditions.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Fundamental Understanding of Transport Under Reactor Extremes (FUTURE); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)

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

OSTI ID:: 2432322

Alternate ID(s):: OSTI ID: 2438493

Report Number(s):: LA-UR--24-21620; PNNL-SA--195013

Journal Information:: Materialia, Journal Name: Materialia Vol. 34; ISSN 2589-1529

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (46)

Applications of the FIB lift-out technique for TEM specimen preparation Giannuzzi, Lucille A.; Drown, Jennifer L.; Brown, Steve R. Microscopy Research and Technique, Vol. 41, Issue 4 https://doi.org/10.1002/(SICI)1097-0029(19980515)41:4<285::AID-JEMT1>3.0.CO;2-Q	journal	May 1998
Resolving Diverse Oxygen Transport Pathways Across Sr-Doped Lanthanum Ferrite and Metal-Perovskite Heterostructures Taylor, Sandra D.; Yano, Kayla H.; Sassi, Michel Advanced Materials Interfaces, Vol. 10, Issue 7 https://doi.org/10.1002/admi.202202276	journal	January 2023
Synthesis, Properties, and Applications of Iron Nanoparticles Huber, Dale?L. Small, Vol. 1, Issue 5 https://doi.org/10.1002/smll.200500006	journal	May 2005
Grain boundary self-diffusion in Fe films with a stable nanostructure Schmidt, H.; Chakravarty, S.; Jiang, M. Journal of Materials Science, Vol. 47, Issue 9 https://doi.org/10.1007/s10853-012-6262-0	journal	January 2012
Molecular dynamics simulation of iron nanoparticle sintering during flame synthesis Nguyen, Ngoc Ha; Henning, Richter; Wen, John Z. Journal of Nanoparticle Research, Vol. 13, Issue 2 https://doi.org/10.1007/s11051-010-0082-4	journal	September 2010
Nanoscale Perspectives of Metal Degradation via In Situ Atom Probe Tomography Lambeets, Sten V.; Kautz, Elizabeth J.; Wirth, Mark G. Topics in Catalysis https://doi.org/10.1007/s11244-020-01367-z	journal	September 2020
Erratum to: Overview of SIMS-Based Experimental Studies of Tracer Diffusion in Solids and Application to Mg Self-Diffusion Kulkarni, Nagraj S.; Bruce Warmack, Robert J.; Radhakrishnan, Bala Journal of Phase Equilibria and Diffusion, Vol. 35, Issue 6 https://doi.org/10.1007/s11669-014-0352-4	journal	October 2014
Modeling and Simulation of Sintering Process Across Scales Yi, Min; Wang, Wenxuan; Xue, Ming Archives of Computational Methods in Engineering, Vol. 30, 3325-3358 https://doi.org/10.1007/s11831-023-09905-0	journal	March 2023
Self diffusion in iron Buffington, F. S.; Hirano, K.; Cohen, M. Acta Metallurgica, Vol. 9, Issue 5 https://doi.org/10.1016/0001-6160(61)90137-7	journal	May 1961
Self-diffusion in ferromagnetic α-iron Hettich, G.; Mehrer, H.; Maier, K. Scripta Metallurgica, Vol. 11, Issue 9 https://doi.org/10.1016/0036-9748(77)90078-3	journal	September 1977
A measurement of surface diffusion across steps on a curved surface (Pd on W) Roux, H.; Piquet, A.; Uzan, R. Surface Science, Vol. 141, Issue 1 https://doi.org/10.1016/0039-6028(84)90212-7	journal	June 1984
Temperature dependence of surface self-diffusion on Pt(001) Kellogg, G. L. Surface Science, Vol. 246, Issue 1-3 https://doi.org/10.1016/0039-6028(91)90388-9	journal	April 1991
Surface self-diffusion of Si on Si(001) Mo, Y. -W.; Kleiner, J.; Webb, M. B. Surface Science, Vol. 268, Issue 1-3 https://doi.org/10.1016/0039-6028(92)90968-C	journal	January 1992
Development of a novel SIMS technique for oxygen self-diffusion and surface exchange coefficient measurements in oxides of high diffusivity Chater, R. J.; Carter, S.; Kilner, J. A. Solid State Ionics, Vol. 53-56 https://doi.org/10.1016/0167-2738(92)90266-R	journal	July 1992
A general protocol for the reconstruction of 3D atom probe data Bas, P.; Bostel, A.; Deconihout, B. Applied Surface Science, Vol. 87-88 https://doi.org/10.1016/0169-4332(94)00561-3	journal	March 1995
Grain boundary self-diffusion in high purity iron Inoue, A.; Nitta, H.; Iijima, Y. Acta Materialia, Vol. 55, Issue 17 https://doi.org/10.1016/j.actamat.2007.06.041	journal	October 2007
Temperature-dependent surface free energy and the Wulff shape of iron and iron carbide nanoparticles: A molecular dynamics study Xing, Mengjiao; Pathak, Amar-Deep; Sanyal, Suchismita Applied Surface Science, Vol. 509 https://doi.org/10.1016/j.apsusc.2019.144859	journal	November 2019
Simulated surface diffusion in nanoporous gold and its dependence on surface curvature Winkeljohn, Conner Marie; Shahriar, Sadi; Seker, Erkin Computational Materials Science, Vol. 230 https://doi.org/10.1016/j.commatsci.2023.112430	journal	August 2023
Tracer diffusion of Cr in Ni and Ni-22Cr studied by SIMS Gheno, Thomas; Jomard, François; Desgranges, Clara Materialia, Vol. 3 https://doi.org/10.1016/j.mtla.2018.08.004	journal	November 2018
Progress in corrosion science at atomic and nanometric scales Maurice, Vincent; Marcus, Philippe Progress in Materials Science, Vol. 95 https://doi.org/10.1016/j.pmatsci.2018.03.001	journal	June 2018
Embedded-atom potential for Fe and its application to self-diffusion on Fe(100) Chamati, H.; Papanicolaou, N. I.; Mishin, Y. Surface Science, Vol. 600, Issue 9 https://doi.org/10.1016/j.susc.2006.02.010	journal	May 2006
Structural, electronic, and magnetic properties of bcc iron surfaces Błoński, P.; Kiejna, A. Surface Science, Vol. 601, Issue 1 https://doi.org/10.1016/j.susc.2006.09.013	journal	January 2007
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
Wide-Field-of-View Atom Probe Reconstruction Geiser, Bp; Larson, Dj; Oltman, E. Microscopy and Microanalysis, Vol. 15, Issue S2 https://doi.org/10.1017/S1431927609098249	journal	July 2009
Radiation-Enhanced Anion Transport in Hematite Yano, Kayla H.; Kohnert, Aaron A.; Banerjee, Amitava Chemistry of Materials, Vol. 33, Issue 7 https://doi.org/10.1021/acs.chemmater.0c04235	journal	March 2021
Radiation Enhanced Anion Diffusion in Chromia Yano, Kayla H.; Kohnert, Aaron A.; Kaspar, Tiffany C. The Journal of Physical Chemistry C, Vol. 125, Issue 50 https://doi.org/10.1021/acs.jpcc.1c08705	journal	December 2021
Resolving Iron(II) Sorption and Oxidative Growth on Hematite (001) Using Atom Probe Tomography Taylor, Sandra D.; Liu, Jia; Arey, Bruce W. The Journal of Physical Chemistry C, Vol. 122, Issue 7 https://doi.org/10.1021/acs.jpcc.7b11989	journal	February 2018
Adatom-Driven Oxygen Intermixing during the Deposition of Oxide Thin Films by Molecular Beam Epitaxy Kaspar, Tiffany C.; Hatton, Peter; Yano, Kayla H. Nano Letters, Vol. 22, Issue 12 https://doi.org/10.1021/acs.nanolett.2c01678	journal	June 2022
Quantitative Measurement of the Surface Self-Diffusion on Au Nanoparticles by Aberration-Corrected Transmission Electron Microscopy Surrey, A.; Pohl, D.; Schultz, L. Nano Letters, Vol. 12, Issue 12, p. 6071-6077 https://doi.org/10.1021/nl302280x	journal	February 2012
Enhancement of surface self-diffusion of platinum atoms by adsorbed hydrogen Horch, S.; Lorensen, H. T.; Helveg, S. Nature, Vol. 398, Issue 6723 https://doi.org/10.1038/18185	journal	March 1999
Dose rate dependent cation & anion radiation enhanced diffusion in hematite Yano, Kayla H.; Kohnert, Aaron A.; Kaspar, Tiffany C. Journal of Materials Chemistry A, Vol. 2022, Issue 10, 24167-24177 https://doi.org/10.1039/D2TA03403D	journal	November 2022
Surface self-diffusion on an fcc crystal: An atomic view Ayrault, Guy; Ehrlich, Gert The Journal of Chemical Physics, Vol. 60, Issue 1 https://doi.org/10.1063/1.1680781	journal	January 1974
Atomic View of Surface Self‐Diffusion: Tungsten on Tungsten Ehrlich, Gert; Hudda, F. G. The Journal of Chemical Physics, Vol. 44, Issue 3 https://doi.org/10.1063/1.1726787	journal	February 1966
Sintering Crystalline Solids. I. Intermediate and Final State Diffusion Models Coble, R. L. Journal of Applied Physics, Vol. 32, Issue 5 https://doi.org/10.1063/1.1736107	journal	May 1961
Sintering Crystalline Solids. II. Experimental Test of Diffusion Models in Powder Compacts Coble, R. L. Journal of Applied Physics, Vol. 32, Issue 5 https://doi.org/10.1063/1.1736108	journal	May 1961
Direct determination of grain‐boundary and dislocation self‐diffusion coefficients in silver from experiments in type‐C kinetics Sommer, J.; Herzig, Chr. Journal of Applied Physics, Vol. 72, Issue 7 https://doi.org/10.1063/1.352328	journal	October 1992
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
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
On the transition between the C and B kinetic regimes for grain-boundary diffusion Szabó, I. A.; Beke, D. L.; Kedves, F. J. Philosophical Magazine A, Vol. 62, Issue 2 https://doi.org/10.1080/01418619008243919	journal	August 1990
Surface diffusion of metals ‐ a comparison of intrinsic and mass transfer measurements Bonze, H. P. C R C Critical Reviews in Solid State Sciences, Vol. 6, Issue 2 https://doi.org/10.1080/10408437608243554	journal	April 1976
Field-ion microscopy-a review of basic principles and selected applications Panitz, J. A. Journal of Physics E: Scientific Instruments, Vol. 15, Issue 12 https://doi.org/10.1088/0022-3735/15/12/004	journal	December 1982
Self-diffusion and defect annihilation in nanocrystalline Fe films probed by neutron reflectometry Chakravarty, Sujoy; Schmidt, Harald; Tietze, Ursula Physical Review B, Vol. 80, Issue 1 https://doi.org/10.1103/PhysRevB.80.014111	journal	July 2009
Surface self-diffusion on Pt(001) by an atomic exchange mechanism Kellogg, G. L.; Feibelman, Peter J. Physical Review Letters, Vol. 64, Issue 26 https://doi.org/10.1103/PhysRevLett.64.3143	journal	June 1990
Evolution of tip shape during field evaporation of complex multilayer structures: EVOLUTION OF TIP SHAPE DURING FIELD EVAPORATION Marquis, E. A.; Geiser, B. P.; Prosa, T. J. Journal of Microscopy, Vol. 241, Issue 3 https://doi.org/10.1111/j.1365-2818.2010.03421.x	journal	February 2011
Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO ₂ hydrogenation Zhu, Jie; Wang, Peng; Zhang, Xiaoben Science Advances, Vol. 8, Issue 5 https://doi.org/10.1126/sciadv.abm3629	journal	February 2022
Influence of Material and Process Parameters on Reduction-Swelling Characteristics of Sintered Iron Pellets Rane, Kedarnath; Date, Prashant; Srivatsan, T. S. Metals, Vol. 13, Issue 1 https://doi.org/10.3390/met13010141	journal	January 2023

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Directly resolving surface vs. lattice self-diffusion in iron at the nanoscale using in situ atom probe capabilities

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