Zhang Guolun, Yang Chengzhi, Wei Qilin, Long Jiangjie, Shen Xiaodong, Chen Yijun, Ke Bao, Liang Weizheng, Zhong Xianci, Zou Bingsuo
School of Physical Science and Technology, Guangxi University, Nanning 530004, China.
State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, MOE Key Laboratory of New Processing Technology for Nonferrous Metals and Materials, and School of Resources, Environment and Materials, Guangxi University, Nanning 530004, China.
ACS Appl Mater Interfaces. 2024 Jan 24;16(3):3841-3852. doi: 10.1021/acsami.3c15442. Epub 2024 Jan 11.
In recent years, low-dimensional organic-inorganic hybrid metal halides (OIHMHs) have shown excellent photophysical properties due to their quantum structure, adjustable energy levels, and energy transfer between inorganic and organic components, which have attracted extensive attention from researchers. Herein, we synthesize a zero-dimensional (0D) OIHMH, Sb:(Gua)InCl, by introducing Sb into (Gua)InCl, which undergoes a significant enhancement of the emission peak at 580 nm with the photoluminescence quantum yield (PLQY) boosted from 17.86 to 95.72% when excited at 340 nm. This boost in photoluminescence of the doped sample was studied by combining ultrafast femtosecond transient absorption, temperature-dependent photoluminescence (PL) spectra, and density functional theory (DFT) calculation, revealing the process of self-trapped exciton (STE) recombination to emit light at both Sb and In sites in this 0D structure simultaneously. This material with the lowest dark STE level at the In site for emission in the undoped sample can amazingly yield very strong emission in the doped sample, which has never been observed before. Finally, we tested its application in a photoelectric device. This work not only helps to gain a deeper understanding of the formation of STEs in In-based halides but also plays a certain guiding role in the design of new luminescent materials.
近年来，低维有机-无机杂化金属卤化物（OIHMHs）因其量子结构、可调节的能级以及无机和有机组分之间的能量转移而表现出优异的光物理性质，这引起了研究人员的广泛关注。在此，我们通过将Sb引入（Gua）InCl中合成了一种零维（0D）OIHMH，即Sb:(Gua)InCl，当在340nm激发时，其在580nm处的发射峰显著增强，光致发光量子产率（PLQY）从17.86%提高到95.72%。通过结合超快飞秒瞬态吸收、变温光致发光（PL）光谱和密度泛函理论（DFT）计算，研究了掺杂样品光致发光的增强过程，揭示了自陷激子（STE）在该0D结构中的Sb和In位点同时复合发光的过程。这种在未掺杂样品中In位点具有最低暗STE能级用于发光的材料，在掺杂样品中能惊人地产生非常强的发射，这是以前从未观察到的。最后，我们测试了其在光电器件中的应用。这项工作不仅有助于更深入地理解In基卤化物中STE的形成，而且对新型发光材料的设计具有一定的指导作用。
