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Photoluminescence Blinking of Single-Crystal Methylammonium Lead Iodide Perovskite Nanorods Induced by Surface Traps

机译:表面陷阱诱导的单晶体甲基铵碘化钙钛矿钙钛矿纳米棒的光致发光闪烁

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摘要

Photoluminescence (PL) of organometal halide perovskite materials reflects the charge dynamics inside of the material and thus contains important information for understanding the electro-optical properties of the material. Interpretation of PL blinking of methylammonium lead iodide (MAPbI3) nanostructures observed on polycrystalline samples remains puzzling owing to their intrinsic disordered nature. Here, we report a novel method for the synthesis of high-quality single-crystal MAPbI3 nanorods and demonstrate a single-crystal study on MAPbI3 PL blinking. At low excitation power densities, two-state blinking was found on individual nanorods with dimensions of several hundred nanometers. A super-resolution localization study on the blinking of individual nanorods showed that single crystals of several hundred nanometers emit and blink as a whole, without showing changes in the localization center over the crystal. Moreover, both the blinking ON and OFF times showed power-law distributions, indicating trapping-detrapping processes. This is further supported by the PL decay times of the individual nanorods, which were found to correlate with the ON/OFF states. Furthermore, a strong environmental dependence of the nanorod PL blinking was revealed by comparing the measurements in vacuum, nitrogen, and air, implying that traps locate close to crystal surfaces. We explain our observations by proposing surface charge traps that are likely related to under-coordinated lead ions and methylammonium vacancies to result in the PL blinking observed here.
机译:有机金属卤化物钙钛矿材料的光致发光(PL)反映了材料内部的电荷动态,因此包含了重要的信息,以了解该材料的电光特性。在多晶样品上观察到的对甲基铵碘化铅(MAPbI3)纳米结构的PL闪烁的解释由于其固有的无序性而仍然令人费解。在这里,我们报告了一种合成高质量单晶MAPbI3纳米棒的新方法,并展示了MAPbI3 PL闪烁的单晶研究。在低激发功率密度下,在尺寸为几百纳米的单个纳米棒上发现了两个状态的闪烁。对单个纳米棒的闪烁进行的超分辨率定位研究表明,数百纳米的单晶整体上会发光并闪烁,而没有显示出晶体上的定位中心发生变化。此外,闪烁的开和关时间均显示了功率定律分布,表明了捕集-捕集过程。单个纳米棒的PL衰减时间进一步支持了这一点,发现该衰减时间与ON / OFF状态相关。此外,通过比较真空,氮气和空气中的测量值,揭示了纳米棒PL闪烁的强烈的环境依赖性,这意味着陷阱位于晶体表面附近。我们通过提出可能与未配位的铅离子和甲基铵空位有关的表面电荷陷阱来解释我们的观察结果,从而导致此处观察到的PL闪烁。

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