Emergence of Ruddlesden-Popper phases and other pitfalls for moderate temperature solution deposited chalcogenide perovskites

Chalcogenide perovskites have recently attracted significant attention for renewable energy applications due to their predicted combination of air, moisture, and thermal stability, which has been experimentally validated, along with their excellent optoelectronic properties, which are still under ex...

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Veröffentlicht in:Materials chemistry frontiers 2024-10, Vol.8 (2), p.3358-3372
Hauptverfasser: Pradhan, Apurva A, Agarwal, Shubhanshu, Vincent, Kiruba Catherine, Hayes, Daniel C, Peterson, Jonas M, Turnley, Jonathan W, Spilker, Robert M, Uible, Madeleine C, Bart, Suzanne C, Huang, Libai, Kisslinger, Kim, Agrawal, Rakesh
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Sprache:eng
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Zusammenfassung:Chalcogenide perovskites have recently attracted significant attention for renewable energy applications due to their predicted combination of air, moisture, and thermal stability, which has been experimentally validated, along with their excellent optoelectronic properties, which are still under experimental investigation. While historically requiring high synthesis temperatures, some solution-processed routes have recently emerged for synthesizing chalcogenide perovskites, such as BaZrS 3 and BaHfS 3 , at temperatures below 600 °C. This study discusses several experimental challenges associated with the moderate-temperature synthesis of solution-deposited chalcogenide perovskites. Firstly, we identify Ruddlesden-Popper (RP) phases as thermodynamically stable competing secondary phases in perovskite synthesis. High sulfur pressures favor the formation of BaZrS 3 or BaHfS 3 , whereas lower sulfur pressures result in a mixture of perovskite and RP phases. Additionally, we briefly discuss the mechanism of moderate-temperature synthesis of chalcogenide perovskites, including some of the morphological and optoelectronic challenges it presents, such as grain overgrowth, secondary phase contamination entrapment, and the presence of mid-band gap emissions. Finally, we address the importance of substrate selection and the potential presence of Ca- and Na-based impurities originating from cation out-diffusion from glass substrates. Addressing these challenges will be crucial as these unique materials continue to be investigated for applications in optoelectronic devices. This work highlights the challenges of weak photoluminescence, the limited choice of substrates, unwanted impurity phases, and Ruddlesden-Popper phases in the moderate-temperature synthesized chalcogenide perovskites.
ISSN:2052-1537
2052-1537
DOI:10.1039/d4qm00441h