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Machine Learning Automated Analysis of Enormous Synchrotron X-ray Diffraction Datasets
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    C: Spectroscopy and Dynamics of Nano, Hybrid, and Low-Dimensional Materials

    Machine Learning Automated Analysis of Enormous Synchrotron X-ray Diffraction Datasets
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    • Xiaodong Zhao
      Xiaodong Zhao
      Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      Department of Chemistry, Washington State University, Pullman 99164, United States
    • YiXuan Luo
      YiXuan Luo
      Department of Electrical and Computer Engineering, University of Rochester, New York 14627, United States
      More by YiXuan Luo
    • Juejing Liu
      Juejing Liu
      Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      Materials Science and Engineering Program, Washington State University, Pullman 99164, United States
      More by Juejing Liu
    • Wenjun Liu
      Wenjun Liu
      Advanced Photon Source, Argonne National Laboratory, Lemont 60439, United States
      More by Wenjun Liu
    • Kevin M. Rosso
      Kevin M. Rosso
      Pacific Northwest National Laboratory, Richland, Washington 99354, United States
    • Xiaofeng Guo*
      Xiaofeng Guo
      Department of Chemistry, Washington State University, Pullman 99164, United States
      Materials Science and Engineering Program, Washington State University, Pullman 99164, United States
      *[email protected]
      More by Xiaofeng Guo
    • Tong Geng*
      Tong Geng
      Department of Electrical and Computer Engineering, University of Rochester, New York 14627, United States
      *[email protected]
      More by Tong Geng
    • Ang Li*
      Ang Li
      Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      *[email protected]
      More by Ang Li
    • Xin Zhang*
      Xin Zhang
      Pacific Northwest National Laboratory, Richland, Washington 99354, United States
      *[email protected]
      More by Xin Zhang
    Other Access OptionsSupporting Information (1)

    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2023, 127, 30, 14830–14838
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    https://doi.org/10.1021/acs.jpcc.3c03572
    Published July 23, 2023
    Copyright © 2023 American Chemical Society

    Abstract

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    X-ray diffraction (XRD) data analysis can be a time-consuming and laborious task. Deep neural network (DNN) based models trained with synthetic XRD patterns have been proven to be a highly efficient, accurate, and automated method for analyzing common XRD data collected from solid samples in ambient environments. However, it remains unclear whether synthetic XRD-based models can be effective in solving micro(μ)-XRD mapping data for in situ experiments involving liquid phases, which always have lower quality and significant artifacts. In this study, we collected μ-XRD mapping data from a LaCl3-calcite hydrothermal fluid system and trained two categories of models to analyze the experimental XRD patterns. The models trained solely with synthetic XRD patterns showed low accuracy (as low as 64%) when solving experimental μ-XRD mapping data. However, the accuracy of the DNN models significantly improved (90% or above) when we trained them with a data set containing both synthetic and a small number of labeled experimental μ-XRD patterns. This study highlights the importance of labeled experimental patterns in training DNN models to solve μ-XRD mapping data from in situ experiments involving liquid phases.

    Copyright © 2023 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcc.3c03572.

    • Architecture of convolution neural network used in binary classification and architecture of convolution neural network used in retrieving phase type and ratio; an illustration of a typical confusion matrix; the schematic representation of the synchrotron XRD data collection and processing progress; representations of the theoretical XRD pattern and comparison between the experimental and theoretical XRD patterns; results of DNN model predicted material phases with training sets with and without experimental data (PDF)

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    Cited By

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    This article is cited by 6 publications.

    1. Litao Chen, Bingxu Wang, Wentao Zhang, Shisheng Zheng, Zhefeng Chen, Mingzheng Zhang, Cheng Dong, Feng Pan, Shunning Li. Crystal Structure Assignment for Unknown Compounds from X-ray Diffraction Patterns with Deep Learning. Journal of the American Chemical Society 2024, 146 (12) , 8098-8109. https://doi.org/10.1021/jacs.3c11852
    2. Yanfei Li, Juejing Liu, Xiaodong Zhao, Wenjun Liu, Tong Geng, Ang Li, Xin Zhang. Accurate and Data‐Efficient Micro X‐ray Diffraction Phase Identification Using Multitask Learning: Application to Hydrothermal Fluids. Advanced Intelligent Systems 2024, 6 (12) https://doi.org/10.1002/aisy.202400204
    3. Avon Datta, Wasif Al Wazed Wasi, Fahim Muntasir, Mahdee Nafis. LIME-RAY: What Does a Neural Network See from X-Rays?. 2024, 239-243. https://doi.org/10.1109/ICICT64387.2024.10839703
    4. Ruhil Dongol, Arpan Mukherjee, Jianming Bai, Hubertus J. J. van Dam, Matthew R. Carbone, E. Frits Abell, Hui Zhong, Akhil Tayal, Lu Ma, Ozgenur Kahvecioglu, Krzysztof Z. Pupek, Deyu Lu, Krishna Rajan, Feng Wang. In situ Synchrotron X‐ray Metrology Boosted by Automated Data Analysis for Real‐time Monitoring of Cathode Calcination. Small Methods 2024, 4 https://doi.org/10.1002/smtd.202400181
    5. Fan Zhang, Jan Ilavsky. Bridging length scales in hard materials with ultra-small angle X-ray scattering – a critical review. IUCrJ 2024, 11 (5) , 675-694. https://doi.org/10.1107/S2052252524006298
    6. Rafael Cardoso Rial. AI in analytical chemistry: Advancements, challenges, and future directions. Talanta 2024, 274 , 125949. https://doi.org/10.1016/j.talanta.2024.125949

    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2023, 127, 30, 14830–14838
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpcc.3c03572
    Published July 23, 2023
    Copyright © 2023 American Chemical Society

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