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量子点固体的基底上合成

Synthesis-on-substrate of quantum dot solids.

作者信息

Jiang Yuanzhi, Sun Changjiu, Xu Jian, Li Saisai, Cui Minghuan, Fu Xinliang, Liu Yuan, Liu Yaqi, Wan Haoyue, Wei Keyu, Zhou Tong, Zhang Wei, Yang Yingguo, Yang Jien, Qin Chaochao, Gao Shuyan, Pan Jun, Liu Yufang, Hoogland Sjoerd, Sargent Edward H, Chen Jun, Yuan Mingjian

机构信息

Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Renewable Energy Conversion and Storage Center (RECAST), College of Chemistry, Nankai University, Tianjin, P. R. China.

Haihe Laboratory of Sustainable Chemical Transformations, Tianjin, P. R. China.

出版信息

Nature. 2022 Dec;612(7941):679-684. doi: 10.1038/s41586-022-05486-3. Epub 2022 Dec 21.

Abstract

Perovskite light-emitting diodes (PeLEDs) with an external quantum efficiency exceeding 20% have been achieved in both green and red wavelengths; however, the performance of blue-emitting PeLEDs lags behind. Ultrasmall CsPbBr quantum dots are promising candidates with which to realize efficient and stable blue PeLEDs, although it has proven challenging to synthesize a monodispersed population of ultrasmall CsPbBr quantum dots, and difficult to retain their solution-phase properties when casting into solid films. Here we report the direct synthesis-on-substrate of films of suitably coupled, monodispersed, ultrasmall perovskite QDs. We develop ligand structures that enable control over the quantum dots' size, monodispersity and coupling during film-based synthesis. A head group (the side with higher electrostatic potential) on the ligand provides steric hindrance that suppresses the formation of layered perovskites. The tail (the side with lower electrostatic potential) is modified using halide substitution to increase the surface binding affinity, constraining resulting grains to sizes within the quantum confinement regime. The approach achieves high monodispersity (full-width at half-maximum = 23 nm with emission centred at 478 nm) united with strong coupling. We report as a result blue PeLEDs with an external quantum efficiency of 18% at 480 nm and 10% at 465 nm, to our knowledge the highest reported among perovskite blue LEDs by a factor of 1.5 and 2, respectively.

摘要

在绿色和红色波长下均已实现外部量子效率超过20%的钙钛矿发光二极管(PeLED);然而,蓝色发光PeLED的性能仍滞后。超小的CsPbBr量子点是实现高效且稳定的蓝色PeLED的有前途的候选材料,尽管事实证明合成单分散的超小CsPbBr量子点具有挑战性,并且在浇铸成固体薄膜时难以保持其溶液相性质。在此,我们报告了在衬底上直接合成适当耦合、单分散的超小钙钛矿量子点薄膜的方法。我们开发了能够在基于薄膜的合成过程中控制量子点尺寸、单分散性和耦合的配体结构。配体上的头部基团(具有较高静电势的一侧)提供空间位阻,抑制层状钙钛矿的形成。尾部(具有较低静电势的一侧)通过卤化物取代进行修饰,以增加表面结合亲和力,将所得晶粒尺寸限制在量子限制范围内。该方法实现了高单分散性(半高宽 = 23 nm,发射中心波长为478 nm)以及强耦合。结果,我们报道了在480 nm处外部量子效率为18%、在465 nm处为10%的蓝色PeLED,据我们所知,这分别是钙钛矿蓝色LED中报道的最高效率的1.5倍和2倍。

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