Filling Chlorine Vacancy with Bromine: A Two-Step Hot-Injection Approach Achieving Defect-Free Hybrid Halogen Perovskite Nanocrystals
Xiaochen Wang, Tianxin Bai, Xuan Meng, Sujun Ji, Ruiling Zhang, Daoyuan Zheng, Bin Yang, Junke Jiang, Keli Han, Feng Liu
Abstract
Mixed-halide (Cl and Br) perovskite nanocrystals (NCs) are of particular interest because they hold great potential for use in high-efficiency blue light-emitting diodes (LEDs). Generally, mixed-halide compounds are obtained by either a one-step synthesis with simultaneous addition of both halide precursors or a postsynthetic anion exchange using the opposite halogen. However, both strategies fail to prevent the formation of deep-level Cl vacancy defects, rendering the photoluminescence quantum yields (PLQYs) typically lower than 30%. Here, by optimizing both thermodynamic and kinetic processes, we devise a two-step hot-injection approach, which simultaneously realizes Cl vacancy filling and efficient anion exchange between Cl– and Br–. Both the identity of Br precursors and their injection temperature are revealed to be critical in transforming those highly defective CsPbCl3 NCs to defect-free CsPb(Cl/Br)3. The optimally synthesized NCs exhibit a saturated blue emission at ∼460 nm with a near-unity PLQY and a narrow emission bandwidth of 18 nm, which represents one of the most efficient blue emitters reported so far. The turn-on voltage of the ensuing LEDs is ∼4.0 V, which is lower than those of most other mixed-halide perovskites. In addition, LEDs exhibit a stable electroluminescence peak at 460 nm under a high bias voltage of 8.0 V. We anticipate that our findings will provide new insights into the materials design strategies for producing high-optoelectronic-quality Cl-containing perovskites.