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Exploring the surface chemistry of cesium lead halide perovskite nanocrystals
摘要: Colloidal nanocrystals (NCs) of cesium lead halide perovskites (CsPbX3, X = Cl, Br or I) are emerging as an exciting class of optoelectronic materials, but the retention of their colloidal and structural integrity during isolation, purification and handling still represents a critical issue. The impelling questions concerning their intrinsic chemical instability are connected to the dynamic nature of the bonding between the inorganic surface and the long-chain capping ligands. However, the key aspects of CsPbX3's surface chemistry that directly impact their stability remain elusive. In this contribution, we provide an in-depth investigation of the surface properties of differently composed CsPbX3 NCs, prepared by traditional hot-injection methods. The study, mainly relying on solution NMR spectroscopy, is backed up by elemental analysis as well as morphological, structural and optical investigations. We ascertained that the nature of the ligand adsorption/desorption processes at the NC surface is dependent on its elemental composition, thus explaining the origin of the instability afflicting CsPbI3 NCs. We also evaluated the effect of NC purification as well as of the degradation pathways involving the organic shell on the surface chemistry of CsPbX3 NCs. This study paves the way for new post-functionalization strategies for this promising class of nanomaterials.
关键词: surface chemistry,colloidal stability,degradation pathways,cesium lead halide perovskite nanocrystals,purification,ligand adsorption/desorption,NMR spectroscopy
更新于2025-09-19 17:15:36
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Room-temperature synthesis of Mn2+-doped cesium lead halide perovskite nanocrystals via a transformation doping method
摘要: Currently, Mn2+-doped cesium lead halide perovskite nanocrystals have attracted research interests. Here, we report a novel room-temperature transformation doping method for the synthesis of Mn2+-doped CsPbCl3 and CsPb(Br/Cl)3 nanocrystals. Innovatively, the transformation of Cs4PbX6 (X=Cl, Br) phase which has no excitation emission to CsPbX3 phase which has strong luminescence was used in this mechanism. Simply injecting MnCl2 precursor into Cs4PbX6 solution could result in the full transformation of Cs4PbX6 phase to CsPbX3 phase and Mn2+-doped CsPbCl3 or CsPb(Br/Cl)3 were obtained. The basic idea for the transformation doping method is that MnCl2 can not only drive the transformation of the two structures but also Mn2+ can substitute Pb2+. In this reaction, the concentration of Mn precursor is a key influence factor. Moreover, instead of the ligand of OA, the acetic acid was used in our method. Through the adjustment of the ligand in precursor, not just the photoluminescence quantum yields of as-prepared Mn2+-doped CsPbCl3 nanocrystals were improved from 7.8 to 32.6% (Mn2+-doped CsPb(Br/Cl)3 nanocrystals even could reach to 42.7%), the nanocrystals also retained outstanding stability. We propose a combination of structure transformation and ion doping as a perovskite doping mechanism. Our doping method is a novel strategy for lead halide perovskite nanocrystals doping project and it could provide more possibilities in the future.
关键词: photoluminescence quantum yields,Cs4PbX6,Mn2+-doped cesium lead halide perovskite nanocrystals,CsPbX3,room-temperature transformation doping method
更新于2025-09-09 09:28:46