期刊
NANOSCALE
卷 13, 期 9, 页码 4899-4910出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0nr08697e
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资金
- National Key R&D program of China [2019YFA0709101, 2016YFB0701003]
- Youth Innovation Promotion Association, CAS [2017272]
- Key Program of the Frontier Science of the Chinese Academy of Sciences [YZDY-SSW-JSC018]
- Fund for Creative Research Groups [21221061]
A method for high-quality alpha-CsPbX3 synthesis at ambient conditions is developed in this study, allowing for simple tuning of size and spectral properties of CsPbX3 nanocrystals by changing cationic ligands or reaction solvents. Additionally, the synthesis of two CsPbX3 materials previously unreported in literature was achieved using this method.
Cubic phase CsPbX3 nanocrystals (NCs) are promising candidates for optoelectronic applications. However, their chemical stability heavily depends on the dynamic ionic surface. In this work, based on the interdependency of the ligands and the reaction solvent, a protocol is developed for high-quality alpha-CsPbX3 under ambient conditions. Utilizing this method, the size and full width at half maximum of CsPbX3 NCs can be simply tuned via changing the cationic ligands or reaction solvent, such as CH3Cl, CH2Cl2, or toluene. One remarkable result is the synthesis of cubic CsPbI3 NCs, for which large-scale syntheses have not been reported in the literature except for our method, due to significant phase transition at room temperature. Another result is that we have realized ultrasmall sized CsPbCl3 NCs with emission at 385 nm for the first time. Furthermore, the elimination of reaction solvent (such as ODE, DMSO, DMF) in our protocol reduces the purification-induced surface ligand loss and the irreversible phase transition to a nonfluorescent phase. Our CsPbX3 NCs show near-perfect photoluminescence quantum yield (PL QY) and long-term stability in the presence of moisture. Further characterization demonstrates that all the ligands, whether the initial paired X type or the degenerated hybrid L-X type, remain perfectly passivating on the defect sites throughout.
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