Facile Preparation of Light Emitting Organic Metal Halide Crystals with Near-Unity Quantum Efficiency
Facile Preparation of Light Emitting Organic Metal Halide Crystals with Near-Unity Quantum Efficiency
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DOI：
10.1021/acs.chemmater.8b00129
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发表时间：
2018-03
影响因子：
8.6
通讯作者：
Chenkun Zhou;Michael Worku;J. Neu;Haoran Lin;Yu Tian;Sujin Lee;Yan Zhou;Dan Han;Shiyou Chen-Shiyou-Ch
中科院分区：
文献类型：
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作者：
Chenkun Zhou;Michael Worku;J. Neu;Haoran Lin;Yu Tian;Sujin Lee;Yan Zhou;Dan Han;Shiyou Chen-Shiyou-Ch
我们报道了一种新型的具有零维（0 D）结构的离子键合有机金属卤化物杂化物（Ph 4P）2SbCl 5的合成和表征。通过四苯基磷（Ph 4P+）和氯化锑（Sb 3+）盐的共结晶，可以高收率地制备出（Ph 4P）2SbCl 5块状单晶，其具有高效率的宽带红光发射，峰值位于648 nm，光致发光量子效率（PLQE）约为87%。密度泛函理论（DFT）的计算揭示了发光的起源为磷光的激子定位在SbCl 52-与强烈的激发态结构畸变。有趣的是，（Ph 4P）2SbCl 5块体晶体与PLQE约100%，可以通过快速晶体生长过程中在几分钟内，随后通过自发的结构转变。结果表明，在快速生长过程中，得到了一种黄色的含有溶剂分子的亚稳态产物，该产物在生长过程中变成了红色的发光产物。
We report the synthesis and characterization of (Ph4P)2SbCl5, a novel ionically bonded organic metal halide hybrid with a zero-dimensional (0D) structure at the molecular level. By cocrystallization of tetraphenylphosphonium (Ph4P+) and antimony (Sb3+) chloride salts, (Ph4P)2SbCl5 bulk single crystals can be prepared in high yield, which exhibit a highly efficient broadband red emission peaked at 648 nm with a photoluminescence quantum efficiency (PLQE) of around 87%. Density functional theory (DFT) calculations reveal the origin of emission as phosphorescence from the excitons localized at SbCl52– with strong excited-state structural distortion. Interestingly, (Ph4P)2SbCl5 bulk crystals with a PLQE of around 100% can be prepared via a rapid crystal growth process within minutes, followed by a spontaneous structural transformation. It was found that the rapid growth process yielded a yellow emitting kinetically favored metastable product containing solvent molecules, which turned into the red emitting the...