四元混合金属硫卤化物的热力学可及性如何？

中文摘要 AI 辅助

四元混合金属硫卤化物（MMCHs）是一类有前景的混合阴离子半导体家族，但其热力学可及性在很大程度上仍未得到探索。我们将密度泛函理论与亚历山大材料数据库相结合，对54种M(II)$_2$M(III)Ch$_2$X$_3$化合物的热力学可及性进行了快速且可靠的评估。所有评估的MMCHs均被预测为热力学不稳定，但相当一部分MMCHs处于凸包的计算机不确定性范围内。其预测的分解遵循五种不同的反应路径，最常见的是分解为M(III)$_2$Ch$_3$、M(II)X$_2$和M(II)Ch。对六种基于Sn的MMCHs的溶液处理支持了我们的分析。值得注意的是，这包括首次在复相薄膜中合成了此前未报道的Sn$_2$InS$_2$Br$_3$。我们的方法确定了凸包接近度和竞争相形成是溶液处理过程中MMCH合成可及性的关键约束，从而指导未来的MMCH探索。

英文摘要

Quaternary mixed-metal chalcohalides (MMCHs) are a promising mixed-anion semiconductor family, but their thermodynamic accessibility remains largely unexplored. We combine density functional theory with the Alexandria Materials Database to carry out a rapid and reliable evaluation of the thermodynamic accessibility of 54 M(II)$_2$M(III)Ch$_2$X$_3$ compounds. All evaluated MMCHs are predicted to be thermodynamically unstable, but a considerable fraction of MMCHs lie within computational uncertainty of the convex hull. Their predicted decomposition follows five distinct reaction pathways, most commonly into M(III)$_2$Ch$_3$, M(II)X$_2$, and M(II)Ch. Solution processing of six Sn-based MMCHs supports our analysis. Notably, this includes the first synthesis of the previously unreported Sn$_2$InS$_2$Br$_3$ in a multiphase film. Our approach identifies convex hull proximity and competing phase formation as key constraints on MMCH synthetic accessibility during solution processing, thereby guiding future MMCH exploration.

发表机构

• Aalto University（阿尔托大学）
• Tampere University（坦佩雷大学）
• Xi'an Jiaotong University（西安交通大学）
• Ruhr University Bochum（波鸿鲁尔大学）

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