4.8 Article

Epitaxial Thin Films of a Chalcogenide Perovskite

Journal

CHEMISTRY OF MATERIALS
Volume 33, Issue 18, Pages 7457-7464

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.1c02202

Keywords

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Funding

  1. Army Research Office [W911NF-19-1-0137, W911NF-21-1-0327]
  2. National Science Foundation of the United States [DMR-1810343, 2122071, DMR-2122070]
  3. USC Provost New Strategic Directions for Research Award
  4. National Science Foundation [DMR-1806147]
  5. DOE BES, QIS Infrastructure Development Project Deterministic Placement and Integration of Quantum Defects
  6. U.S. DOE, Office of Science, Basic Energy Sciences Materials Science and Engineering Division (BESMSED)
  7. Division Of Materials Research
  8. Direct For Mathematical & Physical Scien [2122071] Funding Source: National Science Foundation

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This study reports the direct epitaxial thin film growth of chalcogenide perovskite BaZrS3 by pulsed laser deposition, showing smooth film surfaces and strong potential for photovoltaic applications. The films exhibit clear epitaxial relationship with the substrate, and photodetector devices demonstrate fast and efficient photo response, making BaZrS3 a promising candidate for ultrathin front absorbers in tandem solar cells.
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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