Chalcogenide perovskites, including BaZrS3, have been
suggested as highly stable alternatives to halide perovskites. However,
the synthesis of chalcogenide perovskites has proven to be a significant
challenge, often relying on excessively high temperatures and methods
that are incompatible with device integration. In this study, we developed
a solution-based approach to the deposition of BaZrS3.
This method utilizes a combination of a soluble barium thiolate and
nanoparticulate zirconium hydride. Following solution-based deposition
of the precursors and subsequent sulfurization, BaZrS3 can
be obtained at temperatures as low as 500 °C. Furthermore, this
method was extended to other chalcogenide perovskite (BaHfS3) and perovskite-related (BaTiS3) materials.
Chalcogenide perovskites are promising semiconductor materials with attractive optoelectronic properties and appreciable stability, making them enticing candidates for photovoltaics and related electronic applications. Traditional synthesis methods for these materials have long suffered from high‐temperature requirements of 800–1000 °C. However, the recently developed solution processing route provides a way to circumvent this. By utilizing barium thiolate and ZrH2, this method is capable of synthesizing BaZrS3 perovskite at modest temperatures (500–600 °C), generating crystalline domains on the order of hundreds of nanometers in size. Herein, a systematic study of this solution processing route is done to gain a mechanistic understanding of the process and to supplement the development of device quality fabrication methodologies. A barium polysulfide liquid flux is identified as playing a key role in the rapid synthesis of large‐grain BaZrS3 perovskite at modest temperatures. Additionally, this mechanism is successfully extended to the related BaHfS3 perovskite. The reported findings identify viable precursors, key temperature regimes, and reaction conditions that are likely to enable the large‐grain chalcogenide perovskite growth, essential toward the formation of device‐quality thin films.
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