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Predicting Pulsed-Laser Deposition SrTiO3 Homoepitaxy Growth Dynamics Using High-Speed Reflection High-Energy Electron Diffraction
Journal article   Open access   Peer reviewed

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

Yichen Guo, Peter Meisenheimer, Shuyu Qin, Xinqiao Zhang, Julian Goddy, Ramamoorthy Ramesh, Lane W Martin and Joshua C Agar
ACS applied materials & interfaces, v 17(16), pp 24485-24493
08 Apr 2025
PMID: 40196982
Featured in Collection :   Research Supported by Drexel Libraries' OA Programs
url
https://doi.org/10.1021/acsami.4c12655View
Published, Version of Record (VoR)Open Access via Drexel Libraries Read and Publish Program 2025CC BY V4.0 Open

Abstract

pulsed-laser deposition (PLD) reflection high-energyelectron diffraction (RHEED) surface reconstruction kinetics high-speed imaging (>500 Hz) surface termination effects (TiO2, SrO) open-source analysis tools machine learning and autonomous control Laser Physics Machine Learning
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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Collaboration types
Domestic collaboration
Web of Science research areas
Materials Science, Multidisciplinary
Nanoscience & Nanotechnology
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