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华南理工大学 发光材料与器件国家重点实验室, 广东 广州 510641
[ "叶子青(1996-),男,河南驻马店人,硕士生研究生,2018年于湖北大学获得学士学位,主要从事钙钛矿发光材料与器件的研究。 E⁃mail: 201920118081@mail.scut.edu.cn" ]
[ "陈江山(1978-),男,湖南邵阳人,博士,研究员,2006年于中国科学院长春应用化学研究所获得博士学位,主要从事半导体光电材料与器件的研究。E⁃mail: msjschen@scut.edu.cn" ]
收稿日期:2022-05-11,
修回日期:2022-05-30,
纸质出版日期:2022-08-05
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叶子青,张灯亮,段兴兴等.基于氟代苯乙胺有机阳离子的准二维钙钛矿发光二极管[J].发光学报,2022,43(08):1244-1255.
YE Zi-qing,ZHANG Deng-liang,DUAN Xing-xing,et al.Quasi-2D Perovskite Light-emitting Diodes with Fluorophenethylammonium as Organic Cations[J].Chinese Journal of Luminescence,2022,43(08):1244-1255.
叶子青,张灯亮,段兴兴等.基于氟代苯乙胺有机阳离子的准二维钙钛矿发光二极管[J].发光学报,2022,43(08):1244-1255. DOI: 10.37188/CJL.20220194.
YE Zi-qing,ZHANG Deng-liang,DUAN Xing-xing,et al.Quasi-2D Perovskite Light-emitting Diodes with Fluorophenethylammonium as Organic Cations[J].Chinese Journal of Luminescence,2022,43(08):1244-1255. DOI: 10.37188/CJL.20220194.
近年来,钙钛矿发光二极管(PeLEDs)发展非常迅速,其性能得到了大幅提升,而构筑具有量子阱结构的准二维钙钛矿是开发高性能PeLEDs的有效方法之一。大尺寸有机阳离子是构成准二维钙钛矿的关键组分,对调节准二维钙钛矿的薄膜结构和光电性质具有重要作用。本文通过在铯铅卤化物(CsPb
X
3
)钙钛矿中引入两种单氟取代的溴化苯乙胺(
o
⁃FPEABr(邻位取代)和
p
⁃FPEABr(对位取代)),采用无反溶剂的一步法制备了准二维钙钛矿薄膜和发光器件,研究了它们对准二维钙钛矿成相分布和器件性能的影响。研究发现,
p
⁃FPEABr使准二维钙钛矿形成了大量的低维相,特别是具有强激子‐声子耦合的二维相,而高维相含量较少。相反地,
o
⁃FPEABr能够有效地抑制低维相,并促进高维相的形成,有利于降低非辐射复合和提高辐射复合。形成能计算结果显示,基于
p
⁃FPEABr的低维相比基于
o
⁃FPEABr的低维相具有更好的热力学稳定性,导致了准二维钙钛矿中成相分布的差异,表明改变氟原子的取代位置能够调控准二维钙钛矿的结晶动力学过程,进而影响器件的发光性能。基于
o
⁃FPEABr,我们制备出高效的绿光和蓝光PeLEDs。其中绿光器件的最大外量子效率(EQE)达到了10.27%,发光峰位于521 nm;而蓝光器件的最大EQE也达到了8.88%,发光峰位于488 nm。
During the past few years, the performance of perovskite light-emitting diodes(PeLEDs) has been greatly improved. Constructing quasi-2D perovskites with quantum wells is an effective approach to develop high performance PeLEDs. And the organic cations with large size are crucial to quasi-2D perovskites, which play an important role in regulating the film structures and optoelectronic properties of quasi-2D perovskites. Here we incorporated 2-fluorophenethylammonium bromide (
ortho
-substituted
o
-FPEABr) and 4-fluorophenethylammonium bromide(
para
-substituted
p
-FPEABr) into cesium lead halides to prepare quasi-2D perovskite films by one-step method without antisolvent for PeLEDs, and studied the effect of the fluorine substituted organic cations on the phase distribution and device performance. It was found that
p
-FPEABr allowed the quasi-2D perovskites to form abundant low-n phases, especially the 2D phases(
n
=1) with strong exciton-phonon coupling, and a few high-n phases. On the contrary, the incorporation of
o
-FPEABr suppressed the formation of low-n phases and promoted the formation of high-n phases, which is conducive to reduce non-radiative recombination and improve radiative recombination. The determined formation energies indicated that the low-n phases based on
p
-FPEABr show higher thermodynamic stability than those based on
o
-FPEABr, leading to the difference of phase distribution in the quasi-2D perovskite films. This demonstrated that changing the fluorine substituted position in organic cations can regulate the crystallization kinetic of quasi-2D perovskites, and then affect the device performance. Based on
o
-FPEABr, efficient green and blue PeLEDs were fabricated, a green device with emission peak at 521 nm achieved the maximum external quantum efficiency(EQE) of 10.27%, and a blue device with emission peak at 488 nm showed the maximum EQE of 8.88%.
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