Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 31, Issue 45, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202105563
Keywords
chalcogenide perovskites; epitaxy; MBE; semiconductors; thin films
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Funding
- National Science Foundation (NSF) [1751736]
- Office of Naval Research [N00014-18-1-2746]
- Skolkovo Institute of Science and Technology
- NSF Graduate Research Fellowship [1745302]
- Air Force Office of Scientific Research [FA9550-20-0066]
- MIT Research Support Committee
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1751736] Funding Source: National Science Foundation
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The study demonstrates the fabrication of BaZrS3 thin films using MBE, resulting in smooth films on the atomic scale with near-perfect stoichiometry and sharp interfaces. The films grow epitaxially via two competing growth modes, buffered epitaxy and direct epitaxy, showcasing the potential for developing chalcogenide perovskites as semiconductor alloys with tunable properties. This work also signifies a resurgence of gas-source chalcogenide MBE methods.
The making of BaZrS3 thin films by molecular beam epitaxy (MBE) is demonstrated. BaZrS3 forms in the orthorhombic distorted-perovskite structure with corner-sharing ZrS6 octahedra. The single-step MBE process results in films smooth on the atomic scale, with near-perfect BaZrS3 stoichiometry and an atomically sharp interface with the LaAlO3 substrate. The films grow epitaxially via two competing growth modes: buffered epitaxy, with a self-assembled interface layer that relieves the epitaxial strain, and direct epitaxy, with rotated-cube-on-cube growth that accommodates the large lattice constant mismatch between the oxide and the sulfide perovskites. This work sets the stage for developing chalcogenide perovskites as a family of semiconductor alloys with properties that can be tuned with strain and composition in high-quality epitaxial thin films, as has been long-established for other systems including Si-Ge, III-Vs, and II-VIs. The methods demonstrated here also represent a revival of gas-source chalcogenide MBE.
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