2D层状（C 10 H 21 NH 3）2 PbBr 4单晶的激子和约束效应,ACS Applied Energy Materials

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2D层状（C ₁₀ H ₂₁ NH ₃）₂ PbBr ₄单晶的激子和约束效应
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2018-03-20 00:00:00 , DOI: 10.1021/acsaem.7b00265
Huatao Yin ₁ , Lei Jin , Yuqin Qian ₂ , Xia Li ₂ , Yuhao Wu , Michael S. Bowen , Deirdre Kaan , Chao He , Derek I. Wozniak , Bolei Xu , Asa J. Lewis , Weiwei Shen ₃ , Ke Chen , Graham E. Dobereiner , Yan Zhao ₁ , Bradford B. Wayland , Yi Rao ₂

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二维（2D）层状有机-无机铅（II）卤化物材料（C _n H _{2 n +1} NH ₃）₂ PbX ₄（X = I，Br和Cl）的异常光电性能的识别引起了强烈的关注对这类材料的兴趣。2D层状材料（C ₁₀ H ₂₁ NH ₃）₂ PbBr ₄和拟合金（C ₁₀ H ₂₁ NH ₃）₂ PbI ₂ Br _2的单晶生长用于光物理评估。选择10碳烷基铵阳离子进行研究以提供强介电屏蔽，以突出显示阴离子（PbX ₄^2-）半导体层的量子限制效应。2D层状（C ₁₀ H ₂₁ NH ₃）₂ PbBr ₄化合物的单晶表现出特征性的自由激子，其结合能为。280兆电子伏。观察到2.8±0.2 ns的短光致发光寿命表明，基于PbBr ₄的层状材料的这种电子跃迁仅具有单重态。张（C ₁₀ H ₂₁ NH ₃）制备了厚度为几层的₂ PbBr ₄，并通过原子力显微镜实验验证了尺寸。从（C激子排放₁₀ ħ ₂₁ NH ₃）₂ PbBr ₄和（C ₁₀ ħ ₂₁ NH ₃）₂碘化铅₄从本体向下至厚度为五层表现出相对小的光谱偏移指示的10的强烈限制效应-碳烷基铵间隔基。准合金（C ₁₀ H ₂₁ NH ₃）₂ PbBr ₂ I _2的单晶举一个激子吸收峰接近于四溴化的（C ₁₀ ħ ₂₁ NH ₃）₂ PbBr ₄和具有大斯托克斯位移到一个位置类似于四碘化物的发射峰（C ₁₀ ħ ₂₁ NH ₃）₂碘化铅₄。

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Excitonic and Confinement Effects of 2D Layered (C10H21NH3)2PbBr4 Single Crystals

Recognition of unusual optoelectronic properties for two-dimensional (2D) layered organic–inorganic lead(II) halide materials (C_nH_2n+1NH₃)₂PbX₄ (X = I, Br, and Cl) has attracted intense renewed interest in this class of materials. Single crystals of the 2D layered materials (C₁₀H₂₁NH₃)₂PbBr₄ and pseudo-alloy (C₁₀H₂₁NH₃)₂PbI₂Br₂ were grown for photophysical evaluation. A 10-carbon alkylammonium cation was selected for investigation to provide strong dielectric screening in order to highlight quantum confinement effects of the anionic (PbX₄^2–) semiconductor layer. Single crystals of the 2D layered (C₁₀H₂₁NH₃)₂PbBr₄ compound display a characteristic free exciton with a binding energy of ca. 280 meV. Observation of a short photoluminescence lifetime of 2.8 ± 0.2 ns suggests that this electronic transition for the PbBr₄-based layered material has only singlet character. Sheets of (C₁₀H₂₁NH₃)₂PbBr₄ with thicknesses of a few layers were fabricated, and the dimensions were verified by AFM experiments. Excitonic emissions from (C₁₀H₂₁NH₃)₂PbBr₄ and (C₁₀H₂₁NH₃)₂PbI₄ exhibit relatively small spectral shifts from the bulk down to a thickness of five layers indicative of the strong confinement effect of the 10-carbon alkylammonium spacers. Single crystals of the pseudo-alloy (C₁₀H₂₁NH₃)₂PbBr₂I₂ give an excitonic absorption peak close to that of the tetrabromide (C₁₀H₂₁NH₃)₂PbBr₄ and an emission peak with a large Stokes shift to a position similar to that of the tetraiodide (C₁₀H₂₁NH₃)₂PbI₄.

更新日期：2018-03-20

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