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具有高光致发光猝灭温度的基于小有机分子的混合卤化物

Small Organic Molecular-Based Hybrid Halides with High Photoluminescence Quenching Temperature.

作者信息

Zhang Xusheng, Jiang Xingxing, Liu Kunjie, Fan Liubing, Cao Jindong, He Shihui, Wang Na, Zhao Jing, Lin ZheShuai, Liu Quanlin

机构信息

The Beijing Municipal Key Laboratory of New Energy Materials and Technologies, School of Materials Sciences and Engineering, University of Science and Technology Beijing, Beijing 100083, China.

Center for Crystal Research and Development, Key Lab Functional Crystals and Laser Technology of Chinese Academy of Sciences, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, 29, Zhong Guan Cun Dong Lu, Beijing 100190, China.

出版信息

Inorg Chem. 2022 May 16;61(19):7560-7567. doi: 10.1021/acs.inorgchem.2c00711. Epub 2022 May 3.

Abstract

Organic-inorganic metal halides (OIMHs) exhibit excellent photoelectric properties; however, their high-temperature light-emission stability requires further improvement. Here, we report three isostructural OIMHs (CHN)InCl, (CHN)SbCl, and (CHN)SbBr (CHN = dimethylammonium). They are all crystallized in the 222 space group with a zero-dimensional (0D) structure, with orange-red photoluminescence (PL) under 365 nm UV excitation. Among them, (CHN)InCl exhibits the strongest PL with a photoluminescence quantum yield (PLQY) of 13.9% at room temperature. Optical property measurements and density functional theory unveil that the luminescence of (CHN)InCl at 405 and 620 nm is due to free exciton and self-trapped exciton emission, respectively. It is worth noting that (CHN)InCl shows a high PL quenching temperature, maintaining 50% of its room-temperature PL intensity at 425 K, which is rare in OIHMs. This is much higher than the application temperature of phosphors in practical solid-state lighting applications (363-383 K). In this temperature range, the luminous intensity of (CHN)InCl exceeds 60% of that at room temperature. The high PL quenching temperature observed in (CHN)InCl indicates the potential of OIMHs for applications in phosphor-converted light-emitting diodes.

摘要

有机-无机金属卤化物(OIMHs)表现出优异的光电性能;然而,它们的高温发光稳定性仍需进一步提高。在此,我们报道了三种同构的OIMHs:(CH₃NH₃)InCl、(CH₃NH₃)SbCl和(CH₃NH₃)SbBr(CH₃NH₃ = 二甲基铵)。它们均结晶于222空间群,具有零维(0D)结构,在365 nm紫外激发下呈现橙红色光致发光(PL)。其中,(CH₃NH₃)InCl表现出最强的PL,室温下光致发光量子产率(PLQY)为13.9%。光学性质测量和密度泛函理论表明,(CH₃NH₃)InCl在405和620 nm处的发光分别归因于自由激子和自陷激子发射。值得注意的是,(CH₃NH₃)InCl显示出较高的PL猝灭温度,在425 K时保持其室温PL强度的50%,这在OIHMs中很少见。这远高于实际固态照明应用中磷光体的应用温度(363 - 383 K)。在此温度范围内,(CH₃NH₃)InCl的发光强度超过室温下的60%。在(CH₃NH₃)InCl中观察到的高PL猝灭温度表明OIMHs在磷光体转换发光二极管中的应用潜力。

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