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Colloidal Synthesis and Optical Properties of Perovskite-Inspired Cesium Zirconium Halide Nanocrystals
ACS Materials Letters ( IF 9.6 ) Pub Date : 2020-11-11 , DOI: 10.1021/acsmaterialslett.0c00393 Anna Abfalterer 1 , Javad Shamsi 1 , Dominik J. Kubicki 1, 2 , Christopher N. Savory 3 , James Xiao 1 , Giorgio Divitini 4 , Weiwei Li 4 , Stuart Macpherson 1 , Krzysztof Gałkowski 1, 5 , Judith L. MacManus-Driscoll 4 , David O. Scanlon 3, 6 , Samuel D. Stranks 1, 7
ACS Materials Letters ( IF 9.6 ) Pub Date : 2020-11-11 , DOI: 10.1021/acsmaterialslett.0c00393 Anna Abfalterer 1 , Javad Shamsi 1 , Dominik J. Kubicki 1, 2 , Christopher N. Savory 3 , James Xiao 1 , Giorgio Divitini 4 , Weiwei Li 4 , Stuart Macpherson 1 , Krzysztof Gałkowski 1, 5 , Judith L. MacManus-Driscoll 4 , David O. Scanlon 3, 6 , Samuel D. Stranks 1, 7
Affiliation
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Optoelectronic devices based on lead halide perovskites are processed in facile ways, yet are remarkably efficient. There are extensive research efforts investigating lead-free perovskite and perovskite-related compounds, yet there are challenges to synthesize these materials in forms that can be directly integrated into thin film devices rather than as bulk powders. Here, we report on the colloidal synthesis and characterization of lead-free, antifluorite Cs2ZrX6 (X = Cl, Br) nanocrystals that are readily processed into thin films. We use transmission electron microscopy and powder X-ray diffraction measurements to determine their size and structural properties, and solid-state nuclear magnetic resonance measurements reveal the presence of oleate ligand, together with a disordered distribution of Cs surface sites. Density functional theory calculations reveal the band structure and fundamental band gaps of 5.06 and 3.91 eV for Cs2ZrCl6 and Cs2ZrBr6, respectively, consistent with experimental values. Finally, we demonstrate that the Cs2ZrCl6 and Cs2ZrBr6 nanocrystal thin films exhibit tunable, broad white photoluminescence with quantum yields of 45% for the latter, with respective peaks in the blue and green spectral regions and mixed systems exhibiting properties between them. Our work represents a critical step toward the application of lead-free Cs2ZrX6 nanocrystal thin films into next-generation light-emitting applications.
中文翻译：
钙钛矿型铯卤化锆纳米晶的胶体合成及其光学性质
以卤化钙钛矿为基础的光电器件可以方便地进行处理，但是效率却很高。有大量研究工作在研究无铅钙钛矿和钙钛矿相关的化合物，但是以可直接集成到薄膜装置中而不是散装粉末形式的形式合成这些材料仍然存在挑战。在这里，我们报告无铅，抗萤石Cs 2 ZrX 6的胶体合成和表征（X = Cl，Br）纳米晶体，易于加工成薄膜。我们使用透射电子显微镜和粉末X射线衍射测量来确定其尺寸和结构特性，固态核磁共振测量揭示了油酸酯配体的存在以及Cs表面位点的无序分布。密度泛函理论计算揭示了Cs 2 ZrCl 6和Cs 2 ZrBr 6的能带结构和基带隙分别为5.06和3.91 eV ，与实验值一致。最后，我们证明了Cs 2 ZrCl 6和Cs 2 ZrBr 6纳米晶体薄膜表现出可调的，宽泛的白色光致发光，后者的量子产率为45％，蓝色和绿色光谱区域分别具有峰，并且混合体系在它们之间表现出特性。我们的工作代表了将无铅Cs 2 ZrX 6纳米晶体薄膜应用于下一代发光应用的关键一步。
更新日期：2020-12-07
中文翻译：
钙钛矿型铯卤化锆纳米晶的胶体合成及其光学性质
以卤化钙钛矿为基础的光电器件可以方便地进行处理，但是效率却很高。有大量研究工作在研究无铅钙钛矿和钙钛矿相关的化合物，但是以可直接集成到薄膜装置中而不是散装粉末形式的形式合成这些材料仍然存在挑战。在这里，我们报告无铅，抗萤石Cs 2 ZrX 6的胶体合成和表征（X = Cl，Br）纳米晶体，易于加工成薄膜。我们使用透射电子显微镜和粉末X射线衍射测量来确定其尺寸和结构特性，固态核磁共振测量揭示了油酸酯配体的存在以及Cs表面位点的无序分布。密度泛函理论计算揭示了Cs 2 ZrCl 6和Cs 2 ZrBr 6的能带结构和基带隙分别为5.06和3.91 eV ，与实验值一致。最后，我们证明了Cs 2 ZrCl 6和Cs 2 ZrBr 6纳米晶体薄膜表现出可调的，宽泛的白色光致发光，后者的量子产率为45％，蓝色和绿色光谱区域分别具有峰，并且混合体系在它们之间表现出特性。我们的工作代表了将无铅Cs 2 ZrX 6纳米晶体薄膜应用于下一代发光应用的关键一步。
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