Department of Electrical Engineering, ‡Princeton Institute for Science and Technology of Materials, §Department of Chemistry, and ∥Andlinger Center for Energy and the Environment, Princeton University , Princeton, New Jersey 08544, United States.
ACS Nano. 2017 Apr 25;11(4):3957-3964. doi: 10.1021/acsnano.7b00404. Epub 2017 Mar 23.
Hybrid organic-inorganic halide perovskite semiconductors are attractive candidates for optoelectronic applications, such as photovoltaics, light-emitting diodes, and lasers. Perovskite nanocrystals are of particular interest, where electrons and holes can be confined spatially, promoting radiative recombination. However, nanocrystalline films based on traditional colloidal nanocrystal synthesis strategies suffer from the use of long insulating ligands, low colloidal nanocrystal concentration, and significant aggregation during film formation. Here, we demonstrate a facile method for preparing perovskite nanocrystal films in situ and that the electroluminescence of light-emitting devices can be enhanced up to 40-fold through this nanocrystal film formation strategy. Briefly, the method involves the use of bulky organoammonium halides as additives to confine crystal growth of perovskites during film formation, achieving CHNHPbI and CHNHPbBr perovskite nanocrystals with an average crystal size of 5.4 ± 0.8 nm and 6.4 ± 1.3 nm, respectively, as confirmed through transmission electron microscopy measurements. Additive-confined perovskite nanocrystals show significantly improved photoluminescence quantum yield and decay lifetime. Finally, we demonstrate highly efficient CHNHPbI red/near-infrared LEDs and CHNHPbBr green LEDs based on this strategy, achieving an external quantum efficiency of 7.9% and 7.0%, respectively, which represent a 40-fold and 23-fold improvement over control devices fabricated without the additives.
杂化有机-无机卤化物钙钛矿半导体是光电应用(如光伏、发光二极管和激光)的有吸引力的候选材料。钙钛矿纳米晶体尤其受到关注,其中电子和空穴可以在空间上被限制,促进辐射复合。然而,基于传统胶体纳米晶体合成策略的纳米晶体薄膜存在使用长绝缘配体、胶体纳米晶体浓度低以及在薄膜形成过程中严重聚集等问题。在这里,我们展示了一种简便的原位制备钙钛矿纳米晶体薄膜的方法,通过这种纳米晶体薄膜形成策略可以将发光器件的电致发光增强高达 40 倍。简而言之,该方法涉及使用大体积的有机卤化铵作为添加剂,在薄膜形成过程中限制钙钛矿的晶体生长,从而实现 CHNHPbI 和 CHNHPbBr 钙钛矿纳米晶体,其平均晶体尺寸分别为 5.4±0.8nm 和 6.4±1.3nm,这通过透射电子显微镜测量得到了证实。添加剂限制的钙钛矿纳米晶体表现出显著提高的光致发光量子产率和衰减寿命。最后,我们基于该策略展示了高效的 CHNHPbI 红光/近红外 LED 和 CHNHPbBr 绿光 LED,其外量子效率分别达到 7.9%和 7.0%,与没有添加剂制备的对照器件相比,分别提高了 40 倍和 23 倍。