A Low-Temperature Growth Mechanism for Chalcogenide Perovskites
A Low-Temperature Growth Mechanism for Chalcogenide Perovskites
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DOI：
10.1021/acs.chemmater.3c00494
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发表时间：
2023-06
影响因子：
8.6
通讯作者：
Ruiquan Yang;J. Nelson;Calvin Fai;H. A. Yetkin;Chase Werner;Merielle Tervil;Alexander Jess;P. Dale;C. Hages
中科院分区：
文献类型：
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作者：
Ruiquan Yang;J. Nelson;Calvin Fai;H. A. Yetkin;Chase Werner;Merielle Tervil;Alexander Jess;P. Dale;C. Hages
硫系钙钛矿材料由于其独特的光电性能和稳定性，近年来引起了人们越来越多的研究兴趣。然而，这些材料的合成和加工受到对高温和/或长反应时间的需要的限制。在这项工作中，我们解决了一个开放的问题，低温生长机制BaZrS 3。最终，在≥540 °C的温度下，在短短5分钟内证明了使用熔融BaS 3作为助熔剂的BaZrS 3液体辅助生长机制。Zr前体反应性和S（g.）的作用的生长机理和形成的Ba 3 Zr 2S 7进行了讨论，除了纯化所得产品使用一个简单的H2O洗涤。这种生长机制的扩展到其他Ba基硫族化物，包括BaHfS 3，BaNbS 3和BaTiS 3。此外，还提出了一种利用S_2Cl_2在500 °C下生长BaZrS_3的气相传输生长机制。这些结果证明了用于形成硫族化物钙钛矿薄膜的可扩展处理的可行性。
Chalcogenide perovskites have attracted increasing research attention in recent years due to their promise of unique optoelectronic properties combined with stability. However, the synthesis and processing of these materials has been constrained by the need for high temperatures and/or long reaction times. In this work, we address the open question of a low-temperature growth mechanism for BaZrS3. Ultimately, a liquid-assisted growth mechanism for BaZrS3using molten BaS3as a flux is demonstrated at temperatures ≥540 °C in as little as 5 min. The role of Zr-precursor reactivity and S(g.)on the growth mechanism and the formation of Ba3Zr2S7is discussed, in addition to the purification of resulting products using a straightforward H2O wash. The extension of this growth mechanism to other Ba-based chalcogenides is shown, including BaHfS3, BaNbS3, and BaTiS3. In addition, an alternative vapor-transport growth mechanism is presented using S2Cl2for the growth of BaZrS3at temperatures as low as 500 °C in at least 3 h. These results demonstrate the feasibility of scalable processing for the formation of chalcogenide perovskite thin-films.