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.

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This content will become publicly available on Fri Apr 04 00:00:00 EDT 2025

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

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

Grant/Contract Number:: 89233218CNA000001; AC05-79RL01830; AC05-76RL01830

OSTI ID:: 2432322

Alternate ID(s):: OSTI ID: 2438493

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

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

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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