Epitaxial Thin Films of a Chalcogenide Perovskite

Mythili Surendran, Huandong Chen, Boyang Zhao, Arashdeep S. Thind, Shantanu Singh, Thomas Orvis, Huan Zhao, Jae-Kyung Han, Han Htoon, Megumi Kawasaki, Rohan Mishra, and Jayakanth Ravichandran, Chem. Mater. (2021)

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.