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Accelerating Computational Materials Discovery with Machine Learning and Cloud High-Performance Computing: from Large-Scale Screening to Experimental Validation
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    Accelerating Computational Materials Discovery with Machine Learning and Cloud High-Performance Computing: from Large-Scale Screening to Experimental Validation
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    • Chi Chen
      Chi Chen
      Azure Quantum, Microsoft, One Microsoft Way, Redmond, Washington 98052, United States
      More by Chi Chen
    • Dan Thien Nguyen
      Dan Thien Nguyen
      Pacific Northwest National Laboratory, Physical and Computational Sciences Directorate, 902 Battelle Blvd., Richland, Washington 99352, United States
    • Shannon J. Lee
      Shannon J. Lee
      Pacific Northwest National Laboratory, Physical and Computational Sciences Directorate, 902 Battelle Blvd., Richland, Washington 99352, United States
    • Nathan A. Baker
      Nathan A. Baker
      Azure Quantum, Microsoft, One Microsoft Way, Redmond, Washington 98052, United States
    • Ajay S. Karakoti
      Ajay S. Karakoti
      Pacific Northwest National Laboratory, Physical and Computational Sciences Directorate, 902 Battelle Blvd., Richland, Washington 99352, United States
    • Linda Lauw
      Linda Lauw
      Azure Quantum, Microsoft, One Microsoft Way, Redmond, Washington 98052, United States
      More by Linda Lauw
    • Craig Owen
      Craig Owen
      Microsoft Surface, Microsoft, One Microsoft Way, Redmond, Washington 98052, United States
      More by Craig Owen
    • Karl T. Mueller
      Karl T. Mueller
      Pacific Northwest National Laboratory, Physical and Computational Sciences Directorate, 902 Battelle Blvd., Richland, Washington 99352, United States
    • Brian A. Bilodeau
      Brian A. Bilodeau
      Azure Quantum, Microsoft, One Microsoft Way, Redmond, Washington 98052, United States
    • Vijayakumar Murugesan*
      Vijayakumar Murugesan
      Pacific Northwest National Laboratory, Physical and Computational Sciences Directorate, 902 Battelle Blvd., Richland, Washington 99352, United States
      *Email: [email protected]
    • Matthias Troyer*
      Matthias Troyer
      Azure Quantum, Microsoft, One Microsoft Way, Redmond, Washington 98052, United States
      *Email: [email protected]
    Other Access OptionsSupporting Information (1)

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 29, 20009–20018
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    https://doi.org/10.1021/jacs.4c03849
    Published July 9, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    High-throughput computational materials discovery has promised significant acceleration of the design and discovery of new materials for many years. Despite a surge in interest and activity, the constraints imposed by large-scale computational resources present a significant bottleneck. Furthermore, examples of very large-scale computational discovery carried out through experimental validation remain scarce, especially for materials with product applicability. Here, we demonstrate how this vision became reality by combining state-of-the-art machine learning (ML) models and traditional physics-based models on cloud high-performance computing (HPC) resources to quickly navigate through more than 32 million candidates and predict around half a million potentially stable materials. By focusing on solid-state electrolytes for battery applications, our discovery pipeline further identified 18 promising candidates with new compositions and rediscovered a decade’s worth of collective knowledge in the field as a byproduct. We then synthesized and experimentally characterized the structures and conductivities of our top candidates, the NaxLi3–xYCl6 (0≤ x≤ 3) series, demonstrating the potential of these compounds to serve as solid electrolytes. Additional candidate materials that are currently under experimental investigation could offer more examples of the computational discovery of new phases of Li- and Na-conducting solid electrolytes. The showcased screening of millions of materials candidates highlights the transformative potential of advanced ML and HPC methodologies, propelling materials discovery into a new era of efficiency and innovation.

    Copyright © 2024 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/jacs.4c03849.

    • Known compositions rediscovered in this work; elemental compositions from SEM/EDS; and voltage windows, band structures, AIMD conductivity, and the experimental PXRD and Na/Y ratios of the four compounds (PDF)

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    CCDC 23590252359032 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

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    This article is cited by 7 publications.

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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2024, 146, 29, 20009–20018
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.4c03849
    Published July 9, 2024
    Copyright © 2024 American Chemical Society

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