Li Zhongyuan, Song Gaomin, Li Ye, Wang Le, Zhou Tianliang, Lin Zheshuai, Xie Rong-Jun
College of Materials, State Key Laboratory of Physical Chemistry of Solid Surfaces and Fujian Province Key Laboratory of Materials Genome, Xiamen University, Simingnan Road 422, Xiamen 361005, P. R. China.
Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China.
J Phys Chem Lett. 2020 Dec 3;11(23):10164-10172. doi: 10.1021/acs.jpclett.0c03079. Epub 2020 Nov 16.
Low-dimensional metal halide hybrids (OIMHs) have recently been explored as single-component white-light emitters for use in solid-state lighting. However, it still remains challenging to realize tunable white-light emission in lead-free zero-dimensional (0D) hybrid system. Here, a combination strategy has been proposed through doping Sb enabling and balancing multiple emission centers toward the multiband warm white light. We first synthesized a new lead-free 0D (CNH)InBr·HO single crystal, in which isolated [InBr] octahedral units are separated by large organic cations [CNH]. (CNH)InBr·HO exhibits dual-band emissions with one intense cyan emission and a weak red emission tail. The low-energy ultrabroadband red emission tail can be greatly enhanced by the Sb doping. Experimental data and first-principles calculations reveal that the original dominant cyan emission is originated from the organic cations [CNH] and that the broadband red emission is ascribed to self-trapped excitons in [In(Sb)Br]. When the Sb concentration is 0.1%, a single-component warm white-light emission with a photoluminescence quantum efficiency of 23.36%, correlated color temperature of 3347 K, and a color rendering index up to 84 can be achieved. This work represents a significant step toward the realization of single-component white-light emissions in environmental-friendly, high-performance 0D metal halide light-emitting materials.
低维金属卤化物杂化物(OIMHs)最近已被探索用作固态照明中的单组分白光发射体。然而,在无铅零维(0D)混合体系中实现可调谐白光发射仍然具有挑战性。在此,通过掺杂Sb提出了一种组合策略,以实现并平衡多个发射中心,从而实现多波段暖白光发射。我们首先合成了一种新型无铅0D(CNH)InBr·H₂O单晶,其中孤立的[InBr₆]八面体单元被大的有机阳离子[CNH]隔开。(CNH)InBr·H₂O表现出双波段发射,一个是强烈的青色发射和一个微弱的红色发射尾巴。通过Sb掺杂可以大大增强低能量超宽带红色发射尾巴。实验数据和第一性原理计算表明,原来占主导地位的青色发射源自有机阳离子[CNH],而宽带红色发射归因于[In(Sb)Br₆]中的自陷激子。当Sb浓度为0.1%时,可以实现光致发光量子效率为23.36%、相关色温为3347 K且显色指数高达84的单组分暖白光发射。这项工作代表了在环境友好、高性能的0D金属卤化物发光材料中实现单组分白光发射的重要一步。