Electronic mobility, doping, and defects in epitaxial BaZrS3 chalcogenide perovskite thin films

Van Sambeek, Jack; Dong, Jessica; Ievlev, Anton V.; Cai, Tao; Sadeghi, Ida; Jaramillo, R.

doi:10.1063/5.0284663

Electronic mobility, doping, and defects in epitaxial BaZrS₃ chalcogenide perovskite thin films

Journal Article · Mon Aug 25 00:00:00 EDT 2025 · Journal of Applied Physics

DOI:https://doi.org/10.1063/5.0284663· OSTI ID:2587466

^[1]; ^[1]; ^[2]; ^[1]; Sadeghi, Ida ^[1]; ^[1]

Massachusetts Institute of Technology, Cambridge, MA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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 × 10¹⁸ to 4 × 10²⁰ cm⁻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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: Air Force Office of Scientific Research (AFOSR); United States–Israel Binational Science Foundation (BSF); National Science Foundation (NSF); USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2587466

Journal Information:: Journal of Applied Physics, Journal Name: Journal of Applied Physics Journal Issue: 8 Vol. 138; ISSN 0021-8979; ISSN 1089-7550

Publisher:: AIP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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