Wang Jianzhe, Han Chunmiao, Xie Guohua, Wei Ying, Xue Qin, Yan Pengfei, Xu Hui
Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education, School of Chemistry and Materials, Heilongjiang University, 74 Xuefu Road, Harbin 150080 (P.R. China), Fax: (+86) 451-86608042.
Chemistry. 2014 Aug 25;20(35):11137-48. doi: 10.1002/chem.201403244. Epub 2014 Jul 25.
A series of solution-processible electroluminescent (EL) Eu(3+) complexes were constructed with a self-host strategy, in which neutral ligands were employed as functionalized bidentate phosphine oxide (PO) ligands named DPEPOArn (DPEPO = bis(2-(diphenylphosphino)phenyl) ether oxide). The solubility of these complexes was dramatically improved owing to the increased ratios of organic components. This further enhanced the antenna effect of these ligands in both singlet and triplet energy-transfer processes to support high photoluminescent quantum yields (PLQYs) up to 86 % for their Eu(3+) complexes, which is outstanding among conjugated Eu(3+) complexes. Density function theory (DFT) simulations and electrochemical analysis further verified the contributions of DPEPOArn to the carrier injecting/transporting ability of the complexes. In this sense, these functionalized PO ligands served as hosts in optoelectronic processes, which rendered the self-host feature of their Eu(3+) complexes. With the enhanced electrical properties, the spin-coated single-layer organic light-emitting diodes (OLEDs) of these complexes achieved improved low driving voltages, such as onset voltages about 6 V, compared to their Eu(3+)-contained red-emitting polymeric analogues. [Eu(DBM)3DPEPODPNA2] (DBM = 1,3-diphenylpropane-1,3-dione, DPNA = diphenylnaphthylamine) with the most enhanced electrical properties and suitable frontier molecular orbital (FMO) and triplet state locations endowed its devices with the biggest maximum luminance of >90 cd m(-2) and the highest EL efficiencies. This work verified the potential of small molecular EL Eu(3+) complexes for solution-processed OLEDs through rational function integrations.
采用自主体策略构建了一系列可溶液加工的电致发光(EL)铕(III)配合物,其中中性配体被用作功能化双齿氧化膦(PO)配体,命名为DPEPOArn(DPEPO = 双(2 - (二苯基膦基)苯基)醚氧化物)。由于有机成分比例的增加,这些配合物的溶解度显著提高。这进一步增强了这些配体在单线态和三线态能量转移过程中的天线效应,以支持其铕(III)配合物高达86%的高光致发光量子产率(PLQYs),这在共轭铕(III)配合物中是非常突出的。密度泛函理论(DFT)模拟和电化学分析进一步验证了DPEPOArn对配合物载流子注入/传输能力的贡献。从这个意义上说,这些功能化的PO配体在光电过程中充当主体,赋予了其铕(III)配合物自主体特性。随着电学性能的增强,这些配合物的旋涂单层有机发光二极管(OLEDs)实现了更低的驱动电压,例如与含铕(III)的红色发光聚合物类似物相比,起始电压约为6 V。具有最强电学性能、合适的前沿分子轨道(FMO)和三线态位置的[Eu(DBM)3DPEPODPNA2](DBM = 1,3 - 二苯基丙烷 - 1,3 - 二酮,DPNA = 二苯基萘胺)赋予其器件最大亮度>90 cd m(-2)和最高的EL效率。这项工作通过合理的功能整合验证了小分子EL铕(III)配合物用于溶液加工OLEDs的潜力。