Saha Avijit, Yadav Ranjana, Aldakov Dmitry, Reiss Peter
IRIG-SyMMES, Univ. Grenoble Alpes, INP, CEA, CNRS, 38000, Grenoble, France.
Angew Chem Int Ed Engl. 2023 Nov 6;62(45):e202311317. doi: 10.1002/anie.202311317. Epub 2023 Sep 28.
Solution-processed quantum dot (QD) based blue emitters are of paramount importance in the field of optoelectronics. Despite large research efforts, examples of efficient deep blue/near UV-emitting QDs remain rare due to lack of luminescent wide band gap materials and high defect densities in the existing ones. Here, we introduce a novel type of QDs based on heavy metal free gallium sulfide (Ga S ) and their core/shell heterostructures Ga S /ZnS as well as Ga S /ZnS/Al O . The photoluminescence (PL) properties of core Ga S QDs exhibit various decay pathways due to intrinsic defects, resulting in a broad overall PL spectrum. We show that the overgrowth of the Ga S core QDs with a ZnS shell results in the suppression of the intrinsic defect-mediated states leading to efficient deep-blue emission at 400 nm. Passivation of the core/shell structure with amorphous alumina yields a further enhancement of the PL quantum yield approaching 50 % and leads to an excellent optical and colloidal stability. Finally, we develop a strategy for the aqueous phase transfer of the obtained QDs retaining 80 % of the initial fluorescence intensity.
基于溶液处理的量子点(QD)的蓝色发光体在光电子学领域至关重要。尽管进行了大量研究,但由于缺乏发光宽带隙材料以及现有材料中的高缺陷密度,高效的深蓝色/近紫外发光量子点的实例仍然很少。在此,我们介绍一种基于无重金属硫化镓(GaS)及其核/壳异质结构GaS/ZnS以及GaS/ZnS/Al2O3的新型量子点。由于固有缺陷,核心GaS量子点的光致发光(PL)特性表现出各种衰减途径,导致整体PL光谱较宽。我们表明,用ZnS壳层过度生长GaS核心量子点会抑制固有缺陷介导的状态,从而在400 nm处实现高效的深蓝色发射。用非晶氧化铝对核/壳结构进行钝化可进一步提高PL量子产率,接近50%,并导致优异的光学和胶体稳定性。最后,我们开发了一种策略,用于所获得量子点的水相转移,保留了80%的初始荧光强度。