Abstract
We present the electronic transport properties of BaZrS3 thin films grown epitaxially by gas-source molecular beam epitaxy. We observe n-type behavior in all samples, with carrier concentration ranging from 4 × 10 18 to 4 × 10 20 c m − 3 at room temperature (RT). We observe a champion RT Hall mobility of 11.1 cm2 V−1 s−1, which is competitive with established thin-film photovoltaic absorbers. Temperature-dependent Hall mobility data show that phonon scattering dominates at room temperature, in agreement with computational predictions. X-ray diffraction data illustrate a correlation between mobility and antiphase boundary concentration, illustrating how microstructure can affect transport. Despite the well-established environmental stability of chalcogenide perovskites, we observe significant changes to electronic properties as a function of storage time in ambient conditions. With the help of secondary ion mass spectrometry measurements, we propose and support a defect mechanism that explains this behavior: as-grown films have a high concentration of sulfur vacancies that are shallow donors ( V S ⋅ or V S ⋅ ⋅ ) , which are converted into neutral oxygen defects ( O S × ) upon air exposure. We discuss the relevance of this defect mechanism within the larger context of chalcogenide perovskite research, and we identify means to stabilize the electronic properties.
| Original language | English |
|---|---|
| Article number | 085703 |
| Journal | Journal of Applied Physics |
| Volume | 138 |
| Issue number | 8 |
| DOIs | |
| State | Published - Aug 28 2025 |
Funding
This research was supported by the Air Force Office of Scientific Research under Grant No. FA9550-23-1-0695. This research was supported in part by the United States–Israel Binational Science Foundation (BSF) under Grant No. 2020270. This research was supported in part by the National Science Foundation (NSF) under Grant No. DMR-2224948. This research was supported in part by the Sagol Weizmann-MIT Bridge Program. J.V.S. and J.D. acknowledge support from the National Science Foundation Graduate Research Fellowship, Grant No. 1745302. We acknowledge support from AFOSR under Award No. FA9550-23-1-0157. ToF-SIMS characterization was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility, and using instrumentation within ORNL’s Materials Characterization Core provided by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. This work was performed in part at MIT.nano.