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Epitaxial Thin Films of a Chalcogenide Perovskite

  • Mythili Surendran
    Mythili Surendran
    Mork Family Department of Chemical Engineering and Materials Science, University of Southern California, Los Angeles, California 90089, United States
    Core Center for Excellence in Nano Imaging, University of Southern California, Los Angeles, California 90089, United States
  • Huandong Chen
    Huandong Chen
    Mork Family Department of Chemical Engineering and Materials Science, University of Southern California, Los Angeles, California 90089, United States
  • Boyang Zhao
    Boyang Zhao
    Mork Family Department of Chemical Engineering and Materials Science, University of Southern California, Los Angeles, California 90089, United States
    More by Boyang Zhao
  • Arashdeep S. Thind
    Arashdeep S. Thind
    Institute of Materials Science & Engineering, Washington University in St. Louis, St. Louis, Missouri 63130, United States
  • Shantanu Singh
    Shantanu Singh
    Mork Family Department of Chemical Engineering and Materials Science, University of Southern California, Los Angeles, California 90089, United States
  • Thomas Orvis
    Thomas Orvis
    Mork Family Department of Chemical Engineering and Materials Science, University of Southern California, Los Angeles, California 90089, United States
    Core Center for Excellence in Nano Imaging, University of Southern California, Los Angeles, California 90089, United States
    More by Thomas Orvis
  • Huan Zhao
    Huan Zhao
    Center for Integrated Nanotechnologies, Materials Physics and Applications Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States
    More by Huan Zhao
  • Jae-Kyung Han
    Jae-Kyung Han
    School of Mechanical, Industrial & Manufacturing Engineering, Oregon State University, Corvallis, Oregon 97331, United States
  • Han Htoon
    Han Htoon
    Center for Integrated Nanotechnologies, Materials Physics and Applications Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States
    More by Han Htoon
  • Megumi Kawasaki
    Megumi Kawasaki
    School of Mechanical, Industrial & Manufacturing Engineering, Oregon State University, Corvallis, Oregon 97331, United States
  • Rohan Mishra
    Rohan Mishra
    Institute of Materials Science & Engineering, Washington University in St. Louis, St. Louis, Missouri 63130, United States
    Department of Mechanical Engineering & Materials Science, Washington University in St. Louis, St. Louis, Missouri 63130, United States
    More by Rohan Mishra
  • , and 
  • Jayakanth Ravichandran*
    Jayakanth Ravichandran
    Mork Family Department of Chemical Engineering and Materials Science, University of Southern California, Los Angeles, California 90089, United States
    Ming Hsieh Department of Electrical and Computer Engineering, University of Southern California, Los Angeles, California 90089, United States
    *Email: [email protected]
Cite this: Chem. Mater. 2021, 33, 18, 7457–7464
Publication Date (Web):September 13, 2021
https://doi.org/10.1021/acs.chemmater.1c02202
Copyright © 2021 American Chemical Society

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    Abstract

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    Chalcogenide perovskites have emerged as a new class of optoelectronic materials, especially for photovoltaic applications, but fundamental properties and applications of chalcogenide perovskites remain limited due to the lack of high-quality thin films. We report direct epitaxial thin film growth of BaZrS3, a prototypical chalcogenide, by pulsed laser deposition. X-ray diffraction studies show that the films are strongly textured out-of-plane and have a clear in-plane epitaxial relationship with the substrate. Electron microscopy studies confirm the presence of epitaxy for the first few layers of the film at the interface, even though away from the interface, the films are polycrystalline with many extended defects, suggesting the potential for further improvement in growth. X-ray reflectivity and atomic force microscopy show smooth film surfaces and interfaces between the substrate and the film. The films show strong light absorption near the band edge and photoluminescence in the visible region, validating BaZrS3 as a suitable candidate for ultrathin front absorbers in tandem solar cells. The photodetector devices show fast and efficient photo response with the highest ON/OFF ratio reported for BaZrS3 films thus far. Our study opens up opportunities to use high quality thin films of chalcogenide perovskites to probe fundamental physical phenomena in thin films and heterostructures and also in photovoltaic and optoelectronic applications.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.1c02202.

    • HPT sintered BZS target for PLD, temperature dependence on texture, rocking curve, UV–visible spectroscopy, and photodetector measurements (PDF)

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    Cited By

    This article is cited by 12 publications.

    1. Boyang Zhao, Huandong Chen, Ragib Ahsan, Fei Hou, Eric R. Hoglund, Shantanu Singh, Maruda Shanmugasundaram, Huan Zhao, Andrey V. Krayev, Han Htoon, Patrick E. Hopkins, Jan Seidel, Rehan Kapadia, Jayakanth Ravichandran. Photoconductive Effects in Single Crystals of BaZrS3. ACS Photonics 2024, 11 (3) , 1109-1116. https://doi.org/10.1021/acsphotonics.3c01563
    2. Ruiquan Yang, Jessica Nelson, Calvin Fai, Hasan Arif Yetkin, Chase Werner, Merielle Tervil, Alexander D. Jess, Phillip J. Dale, Charles J. Hages. A Low-Temperature Growth Mechanism for Chalcogenide Perovskites. Chemistry of Materials 2023, 35 (12) , 4743-4750. https://doi.org/10.1021/acs.chemmater.3c00494
    3. Corrado Comparotto, Petter Ström, Olivier Donzel-Gargand, Tomas Kubart, Jonathan J. S. Scragg. Synthesis of BaZrS3 Perovskite Thin Films at a Moderate Temperature on Conductive Substrates. ACS Applied Energy Materials 2022, 5 (5) , 6335-6343. https://doi.org/10.1021/acsaem.2c00704
    4. Ji Woon Choi, Byungha Shin, Prashun Gorai, Robert L. Z. Hoye, Robert Palgrave. Emerging Earth-Abundant Solar Absorbers. ACS Energy Letters 2022, 7 (4) , 1553-1557. https://doi.org/10.1021/acsenergylett.2c00516
    5. Apurva A. Pradhan, Madeleine C. Uible, Shubhanshu Agarwal, Jonathan W. Turnley, Shriya Khandelwal, Jonas M. Peterson, Daria D. Blach, Ryan N. Swope, Libai Huang, Suzanne C. Bart, Rakesh Agrawal. Synthesis of BaZrS 3 and BaHfS 3 Chalcogenide Perovskite Films Using Single‐Phase Molecular Precursors at Moderate Temperatures. Angewandte Chemie 2023, https://doi.org/10.1002/ange.202301049
    6. Apurva A. Pradhan, Madeleine C. Uible, Shubhanshu Agarwal, Jonathan W. Turnley, Shriya Khandelwal, Jonas M. Peterson, Daria D. Blach, Ryan N. Swope, Libai Huang, Suzanne C. Bart, Rakesh Agrawal. Synthesis of BaZrS 3 and BaHfS 3 Chalcogenide Perovskite Films Using Single‐Phase Molecular Precursors at Moderate Temperatures. Angewandte Chemie International Edition 2023, https://doi.org/10.1002/anie.202301049
    7. Zhonghai Yu, Chenhua Deng, Sen Kong, Haolei Hui, Jiale Guo, Qizhong Zhao, Fanghua Tian, Chao Zhou, Yin Zhang, Sen Yang, Hao Zeng. Transition metal-doped chalcogenide perovskite magnetic semiconductor B a Z r S 3 . Journal of Magnetism and Magnetic Materials 2022, 563 , 169886. https://doi.org/10.1016/j.jmmm.2022.169886
    8. Mythili Surendran, Boyang Zhao, Guodong Ren, Shantanu Singh, Amir Avishai, Huandong Chen, Jae-Kyung Han, Megumi Kawasaki, Rohan Mishra, Jayakanth Ravichandran. Quasi-epitaxial growth of BaTiS3 films. Journal of Materials Research 2022, 37 (21) , 3481-3490. https://doi.org/10.1557/s43578-022-00776-y
    9. Daniel Zilevu, Omri O. Parks, Sidney E. Creutz. Solution-phase synthesis of the chalcogenide perovskite barium zirconium sulfide as colloidal nanomaterials. Chemical Communications 2022, 58 (75) , 10512-10515. https://doi.org/10.1039/D2CC03494H
    10. Tim Freund, Maria Rita Cicconi, Peter J. Wellmann. Fabrication of Bariumtrisulphide Thin Films as Precursors for Chalcogenide Perovskites. physica status solidi (b) 2022, 259 (9) , 2200094. https://doi.org/10.1002/pssb.202200094
    11. Kevin Ye, Nathan Z. Koocher, Stephen Filippone, Shanyuan Niu, Boyang Zhao, Matthew Yeung, Sharon Bone, Adam J. Robinson, Patrick Vora, André Schleife, Long Ju, Alexey Boubnov, James M. Rondinelli, Jayakanth Ravichandran, R. Jaramillo. Low-energy electronic structure of perovskite and Ruddlesden-Popper semiconductors in the Ba-Zr-S system probed by bond-selective polarized x-ray absorption spectroscopy, infrared reflectivity, and Raman scattering. Physical Review B 2022, 105 (19) https://doi.org/10.1103/PhysRevB.105.195203
    12. Kostiantyn V. Sopiha, Corrado Comparotto, José A. Márquez, Jonathan J. S. Scragg. Chalcogenide Perovskites: Tantalizing Prospects, Challenging Materials. Advanced Optical Materials 2022, 10 (3) , 2101704. https://doi.org/10.1002/adom.202101704

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