DOE OSTI · 3030782
Surface Reordering During Layer‐by‐Layer Growth on SrTiO 3
Abstract
With the development of layer‐by‐layer growth techniques such as molecular beam epitaxy (MBE), it is now possible to construct materials with atomic‐level precision, with the layer sequence primarily determined by the growth recipe. However, materials can still restructure in the high‐temperature growth environment with surface thermodynamics strongly influencing growth behavior. Here, we demonstrate that growth on ${\rm SrTiO}_{3}$ (001), the principal platform for oxide electronics, does not occur in a layer‐by‐layer fashion but follows a more complex process in which a ${\rm TiO}_{2}$ plane continually diffuses toward the growth surface. Employing in situ synchrotron X‐ray scattering combined with ab initio thermodynamic calculations, we discover the existence of a stable ${\rm TiO}_{2}$ double‐layer structure on the pristine substrate and the occurrence of dynamic layer rearrangement during homoepitaxial growth by oxide MBE. Our findings suggest that the current methods used to precisely control ${\rm SrTiO}_{3}$ surfaces are limited, as well as our ability to dictate the composition of ultrathin films, resulting in important ramifications regarding the surface reactivity of perovskite materials grown on ${\rm SrTiO}_{3}$.
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Tung, I‐Cheng [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Northwestern Univ., Evanston, IL (United States)] (ORCID:0000000260931400), Yan, Xi [Argonne National Laboratory (ANL), Argonne, IL (United States)], Lee, June‐Hyuk [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Korea Atomic Energy Research Institute (KAERI), Daejeon (Korea, Republic of)], Liu, Yang [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Zhejiang Univ., Hangzhou (China)], Chang, Seo Hyoung [Argonne National Laboratory (ANL), Argonne, IL (United States)], Luo, Zhenlin [Univ. of Science and Technology of China, Hefei (China)], Wrobel, Friederike [Argonne National Laboratory (ANL), Argonne, IL (United States)], Cheung, Nicholas T. [James Madison Univ., Harrisonburg, VA (United States)], Lopez, Kaden R. [James Madison Univ., Harrisonburg, VA (United States)], Bedzyk, Michael J. [Northwestern Univ., Evanston, IL (United States)], Hong, Hawoong [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)], Freeland, John W. [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)], Zhou, Hua [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)], Letchworth‐Weaver, Kendra [James Madison Univ., Harrisonburg, VA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)], Fong, Dillon D. [Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000159308243). 2026-03-06. Surface Reordering During Layer‐by‐Layer Growth on SrTiO 3. https://doi.org/10.1002/adma.202519431
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