Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN, USA.
Department of Physics, Florida State University, Tallahassee, FL, USA.
Nat Commun. 2023 Jan 25;14(1):397. doi: 10.1038/s41467-023-36118-7.
Electroluminescence efficiencies and stabilities of quasi-two-dimensional halide perovskites are restricted by the formation of multiple-quantum-well structures with broad and uncontrollable phase distributions. Here, we report a ligand design strategy to substantially suppress diffusion-limited phase disproportionation, thereby enabling better phase control. We demonstrate that extending the π-conjugation length and increasing the cross-sectional area of the ligand enables perovskite thin films with dramatically suppressed ion transport, narrowed phase distributions, reduced defect densities, and enhanced radiative recombination efficiencies. Consequently, we achieved efficient and stable deep-red light-emitting diodes with a peak external quantum efficiency of 26.3% (average 22.9% among 70 devices and cross-checked) and a half-life of ~220 and 2.8 h under a constant current density of 0.1 and 12 mA/cm, respectively. Our devices also exhibit wide wavelength tunability and improved spectral and phase stability compared with existing perovskite light-emitting diodes. These discoveries provide critical insights into the molecular design and crystallization kinetics of low-dimensional perovskite semiconductors for light-emitting devices.
二维卤化物钙钛矿的电致发光效率和稳定性受到多量子阱结构形成的限制,这些结构具有较宽且不可控的相分布。在这里,我们报告了一种配体设计策略,可以大大抑制扩散限制的相歧化,从而实现更好的相控制。我们证明,扩展π共轭长度和增加配体的截面积,可以使钙钛矿薄膜具有显著抑制离子输运、变窄的相分布、降低缺陷密度和增强辐射复合效率。因此,我们实现了高效稳定的深红光发光二极管,其峰值外量子效率为 26.3%(70 个器件中平均为 22.9%,经过交叉验证),在 0.1 和 12 mA/cm 的恒定电流密度下的半衰期分别约为 220 和 2.8 小时。与现有钙钛矿发光二极管相比,我们的器件还表现出宽波长可调谐性以及改善的光谱和相稳定性。这些发现为用于发光器件的低维钙钛矿半导体的分子设计和结晶动力学提供了重要的见解。