Lee YuJin, Jo Dae-Yeon, Kim Taehee, Jo Jung-Ho, Park Jumi, Yang Heesun, Kim Dongho
Department of Chemistry, Yonsei University, 50 Yonsei-ro, Seodaemun-gu, Seoul 03722, Republic of Korea.
Department of Materials Science and Engineering, Hongik University, 94 Wausan-ro, Mapo-gu, Seoul 04066, Republic of Korea.
ACS Appl Mater Interfaces. 2022 Mar 16;14(10):12479-12487. doi: 10.1021/acsami.1c20088. Epub 2022 Mar 3.
The main issue in developing a quantum dot light-emitting diode (QLED) display lies in successfully replacing heavy metals with environmentally benign materials while maintaining high-quality device performance. Nonradiative Auger recombination is one of the major limiting factors of QLED performance and should ideally be suppressed. This study scrutinizes the effects of the shell structure and composition on photoluminescence (PL) properties of InP/ZnSeS/ZnS quantum dots (QDs) through ensemble and single-dot spectroscopic analyses. Employing gradient shells is discovered to suppress Auger recombination to a high degree, allowing charged QDs to be luminescent comparatively with neutral QDs. The "lifetime blinking" phenomenon is observed as evidence of suppressed Auger recombination. Furthermore, single-QD measurements reveal that gradient shells in QDs reduce spectral diffusion and elevate the energy barrier for charge trapping. Shell composition dependency in the gradience effect is observed. An increase in the ZnS composition (ZnS >50%) in the gradient shell introduces lattice mismatch between the core and the shell and therefore rather reverses the effect and reduces the QD performance.
开发量子点发光二极管(QLED)显示器的主要问题在于,在保持高质量器件性能的同时,成功地用环境友好型材料替代重金属。非辐射俄歇复合是QLED性能的主要限制因素之一,理想情况下应予以抑制。本研究通过系综和单量子点光谱分析,仔细研究了壳层结构和组成对InP/ZnSeS/ZnS量子点(QD)光致发光(PL)特性的影响。研究发现,采用梯度壳层可在很大程度上抑制俄歇复合,使带电量子点与中性量子点相比能够发光。观察到“寿命闪烁”现象,作为俄歇复合受到抑制的证据。此外,单量子点测量结果表明,量子点中的梯度壳层可减少光谱扩散,并提高电荷俘获的能垒。观察到梯度效应中壳层组成的依赖性。梯度壳层中ZnS组成的增加(ZnS>50%)会导致核与壳之间的晶格失配,从而使效果相反,降低量子点性能。