Low-temperature, solution-based synthesis of chalcogenide perovskites Chuck Hages, Ruiquan Yang, Alex Jess University of Florida, USA Chalcogenide perovskites are an emerging class of semiconductor with the potential to replace the ubiquitous organic-inorganic hybrid metal halide perovskites as a high-performance photovoltaic absorber. This is a result of their predicted enhanced stability, favorable charge transport and absorption properties, and non-toxic nature – while maintaining the defect tolerance and high optoelectronic tunability typical of perovskites. In fact, their stability ultimately results in a high crystallization energy barrier for their formation. As a result, current syntheses fail to realize the potential of chalcogenide perovskites by requiring high temperatures (c. 1000 °C) and/or long reaction times. Accordingly, there is a significant lack of relevant experimental syntheses of chalcogenide perovskites. Additionally, present synthesis routes limit their amenability to tunable materials chemistry for controlling their material properties and synthesis into thin films. Therefore, a critical need exists to develop a low-temperature, solution-based synthesis route to realize chalcogenide perovskites as a next-generation PV technology. In this work we discuss our results in the low-temperature, solution-based synthesis of sulfide chalcogenide perovskite nanoparticles. Our initial results have focused on the synthesis of BaSnS 3 , BaZrS 3 , and BaHfS 3 (and related stoichiometries) as a proof-of-concept for the generalized solution-based synthesis of chalcogenide perovskite nanoparticles. Our research has focused on developing single-source precursors for Ba-S, Zr-S, Hf-S, and Sn-Sn with high-stability (from oxidation), favorable solubility, and low-decomposition temperature (<200 °C); these precursors are based on metal-thiocarbamate complexes. Nanoparticle synthesis of chalcogenide perovskites (and related stoichiometries) have been demonstrated in temperature ranges from 150 – 275 °C. In addition to synthesis, we will discuss structural stability of various synthesis products, use of our low-temperature metal-thiocarbamate complexes for the direct formation of thin films via low-temperature & reactive annealing, and the potential of chalcogenide perovskite nanoparticles in the grain-growth of thin films via reactive annealing.
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