Yan Danni,Dong Yuhui,Wei Naiwei,Yang Shuai,Zhu Hong,Gu Wanzhong,Zou Yousheng,Zeng Haibo
Quaternary Ag-In-Ga-S (AIGS) quantum dot (QD) is considered a promising, spectral-tunable, and environmentally friendly luminescent display material. However, the more complex surface defect states of AIGS QDs resulting from the coexistence of multiple elements lead to a low (< 60%) photoluminescence quantum yield (PLQY). Here, we develop a novel convenient method to introduce Z-type ligands ZnX 2 (X = Cl, Br, I) for passivating the surface defects of AIGS QDs to dramatically enhance the PLQY and stability without affecting the crystalline structure and morphology. Results show that the addition of ZnCl 2 during the purified process of AIGS QDs leads to a 3-fold increase of PLQY (from 28.5% to 87%). Impressively, the highest PLQY is up to a recorded value of 92%, which is comparable to typical heavy metal QDs. Exciton dynamics studies have shown that the rapid annihilation process of excitons in treated QDs is inhibited. We also confirm that the improvement in PLQY is a result of the effective passivation of the non-coordinating atom on the QD surface by building a new bonding between sulfur dangling and Zn 2+ . The realization of high PLQY will further promote the application of AIGS QDs in luminescent displays.
I–III–VI quantum dots (QDs) and derivatives (I, III, and VI are Ag+/Cu+, Ga3+/In3+, and S2–/Se2–, respectively) are the ideal candidates to replace II–VI (e.g., CdSe) and perovskite QDs due to their nontoxicity, pure color, high photoluminescence quantum yield (PLQY), and full visible coverage. However, the chaotic cation alignment in multielement systems can easily lead to the formation of multiple surface vacancies, highlighted as VI and VVI, leading to nonradiative recombination and nonequilibrium carrier distribution, which severely limit the performance improvement of materials and devices. Here, based on Zn–Ag–In–Ga–S QDs, we construct an ultrathin indium sulfide shell that can passivate electron vacancies and convert donor/acceptor level concentrations. The optimized In-rich 2-layer indium sulfide structure not only enhances the radiative recombination rate by preventing further VS formation but also achieves the typical DAP emission enhancement, achieving a significant increase in PLQY to 86.2% at 628 nm. Moreover, the optimized structure can mitigate the lattice distortion and make the carrier distribution in the interior of the QDs more balanced. On this basis, red QD light-emitting diodes (QLEDs) with the highest external quantum efficiency (EQE; 5.32%) to date were obtained, providing a novel scheme for improving I–III–VI QD-based QLED efficiency.