Predicting Pulsed-Laser Deposition SrTiO3 Homoepitaxy Growth Dynamics Using High-Speed Reflection High-Energy Electron Diffraction

Guo, Yichen; Meisenheimer, Peter; Qin, Shuyu; Zhang, Xinqiao; Goddy, Julian; Ramesh, Ramamoorthy; Martin, Lane W.; Agar, Joshua

doi:10.1021/acsami.4c12655

Predicting Pulsed-Laser Deposition SrTiO₃ Homoepitaxy Growth Dynamics Using High-Speed Reflection High-Energy Electron Diffraction

Journal Article · Tue Apr 08 00:00:00 EDT 2025 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.4c12655· OSTI ID:2550689

^[1]; ^[2]; Qin, Shuyu ^[3]; Zhang, Xinqiao ^[4]; ^[4]; Ramesh, Ramamoorthy ^[5]; Martin, Lane W. ^[6]; ^[4]

Lehigh Univ., Bethlehem, PA (United States); Drexel Univ., Philadelphia, PA (United States)
University of California, Berkeley, CA (United States)
Lehigh Univ., Bethlehem, PA (United States)
Drexel Univ., Philadelphia, PA (United States)
Rice Univ., Houston, TX (United States)
University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Rice Univ., Houston, TX (United States)

Pulsed-laser deposition (PLD) is a powerful technique for growing complex oxides with controlled stoichiometry. To understand growth dynamics therein, it is common to leverage in situ spectroscopies, such as reflection high-energy electron diffraction (RHEED), to monitor surface crystallinity. Most commercial systems rely on video-rate cameras operating at 60-120 Hz that lack sufficient temporal resolution to capture growth dynamics at practical deposition frequencies. Here, a high-speed platform to record in situ dynamics via RHEED at >500 Hz is implemented. An open-source analysis package is designed to fit diffraction spots to 2D Gaussians, allowing single-pulse surface reconstruction kinetics extraction. Using homoepitaxially deposited (001)-oriented SrTiO₃ as a model system, we demonstrate how high-speed RHEED can provide real-time insight into growth processes obscured by slower acquisition systems. By fitting the single-pulse intensity to a set of exponential functions, we observe changes in the characteristic decay time and mechanism correlated to the substrate step width and surface termination. We observe distinct surface effects, with diffraction intensity decaying on lower-energy TiO₂-terminated surfaces and stabilizing on SrO- or mixed-terminated surfaces. Similarly, using an exponential model, the extracted characteristic time of adatom deposition decreases with increased density of bonding sites associated with mixed termination and narrower step widths. Ultimately, this work shows how increasing RHEED temporal resolution can uncover new insights into growth processes, with practical implications for the design and control of PLD processes. This experimental platform provides new capabilities to enable data-driven machine learning analysis and autonomous control systems to enhance the complexity and fecundity of PLD.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); US Army Research Office (ARO); USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR)

Grant/Contract Number:: SC0002501

OSTI ID:: 2550689

Alternate ID(s):: OSTI ID: 2568057

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 16 Vol. 17; ISSN 1944-8244; ISSN 1944-8252

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
high-speed imaging (>500 Hz)
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open-source analysis tools
pulsed-laser deposition (PLD)
reflection high-energy electron diffraction (RHEED)
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Predicting Pulsed-Laser Deposition SrTiO3 Homoepitaxy Growth Dynamics Using High-Speed Reflection High-Energy Electron Diffraction

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Predicting Pulsed-Laser Deposition SrTiO₃ Homoepitaxy Growth Dynamics Using High-Speed Reflection High-Energy Electron Diffraction