Colloidal Synthesis and Optical Properties of Perovskite-Inspired Cesium Zirconium Halide Nanocrystals.
Colloidal Synthesis and Optical Properties of Perovskite-Inspired Cesium Zirconium Halide Nanocrystals.
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DOI：
10.1021/acsmaterialslett.0c00393
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发表时间：
2020-12-07
影响因子：
11.4
通讯作者：
Stranks SD
中科院分区：
文献类型：
--
作者：
Abfalterer A;Shamsi J;Kubicki DJ;Savory CN;Xiao J;Divitini G;Li W;Macpherson S;Gałkowski K;MacManus-Driscoll JL;Scanlon DO;Stranks SD
基于卤化铅钙钛矿的光电器件加工简单，但效率很高。人们对无铅钙钛矿和钙钛矿相关化合物进行了广泛的研究，然而，将这些材料合成成可以直接集成到薄膜器件而不是散装粉末的形式存在挑战。在这里，我们报道了无铅反萤石Cs2ZrX6 （X = Cl, Br）纳米晶体的胶体合成和表征，该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它们的尺寸和结构性质，固态核磁共振测量揭示了油酸配体的存在，以及Cs表面位点的无序分布。密度函数理论计算表明，Cs2ZrCl6和Cs2ZrBr6的能带结构和基本带隙分别为5.06和3.91 eV，与实验值一致。最后，我们证明了Cs2ZrCl6和Cs2ZrBr6纳米晶体薄膜表现出可调谐的宽白光致发光，后者的量子产率为45%，在蓝色和绿色光谱区域分别有峰，并且混合系统表现出两者之间的特性。我们的工作代表了将无铅Cs2ZrX6纳米晶体薄膜应用于下一代发光应用的关键一步。
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.
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影响因子：
39.8
作者：
Chen, Min;Ju, Ming-Gang;Padture, Nitin P.
通讯作者：
Padture, Nitin P.
影响因子：
2.8
作者：
DRUMMEN, PJH;DONKER, H;BLASSE, G
通讯作者：
BLASSE, G
影响因子：
3.7
作者：
Kresse, G;Furthmuller, J
通讯作者：
Furthmuller, J
影响因子：
8.6
作者：
Cadars, S.;Smith, B. J.;Chmelka, B. F.
通讯作者：
Chmelka, B. F.
影响因子：
22
作者：
Imran, Muhammad;Ijaz, Palvasha;Manna, Liberato
通讯作者：
Manna, Liberato