Mixed Valence of Bismuth in Hexagonal Chalcohalide Nanocrystals,Chemistry of Materials

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Mixed Valence of Bismuth in Hexagonal Chalcohalide Nanocrystals
Chemistry of Materials ( IF 7.2 ) Pub Date : 2023-01-20 , DOI: 10.1021/acs.chemmater.2c02941
Danila Quarta ₁ , Stefano Toso _{2,

3} , Gabriele Saleh ₂ , Rocco Caliandro ₄ , Anna Moliterni ₄ , Andrea Griesi ₂ , Giorgio Divitini ₂ , Ivan Infante _{2,

5,

6} , Giuseppe Gigli _{1,

7} , Cinzia Giannini ₄ , Liberato Manna ₂ , Carlo Giansante ₁

Affiliation

We report the colloidal synthesis of bismuth chalcohalide nanocrystals, which adopt a hexagonal phase that we describe with the Bi₁₃S₁₈X₂ (in which X = Br and I) structure. Such a model structure displays columns of Bi atoms that form dimers of subvalent Bi (formally Bi₂⁴⁺), which we here ascribe to Peierls-type distortions. We suggest that the Bi₂⁴⁺ dimers are at the origin of the anomalously low band gap of this material, with the lowest energy electronic transition showing analogies with an intervalence charge transfer. Our synthetic approach and insights into the structural and electronic features of the hexagonal bismuth chalcohalides are fundamental to sustain the rapidly increasing use of this class of (nano)materials for diverse applications, such as photocatalysis and thermoelectrics.

中文翻译：

六方卤化物纳米晶中铋的混价

我们报告了卤化铋纳米晶体的胶体合成，该纳米晶体采用我们用 Bi ₁₃ S ₁₈ X ₂（其中 X = Br 和 I）结构描述的六方相。_{这种模型结构显示形成亚价 Bi 二聚体（形式为 Bi 2}⁴⁺ ）的 Bi 原子列，我们在此将其归因于 Peierls 型畸变。我们建议 Bi ₂⁴⁺二聚体是这种材料异常低带隙的起源，最低能量电子跃迁显示与间隔电荷转移的类比。我们的合成方法以及对六方卤化铋的结构和电子特征的深入了解是维持此类（纳米）材料在光催化和热电等各种应用中迅速增加使用的基础。

更新日期：2023-01-20

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