AbstractMn2+ doped CsPbCl3 nanocrystals (Mn2+:CsPbCl3 NCs) show immense promise in lighting and display technologies owing to their outstanding optical characteristics. Nonetheless, high defect density, inefficient Mn2+ doping, and poor structural robustness pose considerable challenges in the synthesis of Mn2+:CsPbCl3 NCs with high photoluminescence quantum yield (PLQY) and long‐term stability. This study introduces an eco‐friendly room‐temperature post‐treatment method utilizing MgCl2/oleylamine solution, boosting the total PLQY of the NCs from 65% to 98%, including a 30% increase for Mn2+ emission. Additionally, the post‐treatment significantly improves the NCs’ resilience against UV light, retaining 80% of their initial PL intensity after 120 hours of UV exposure. Comprehensive analyses including density functional theory simulation and temperature‐dependent PL spectra suggested that the PLQY enhancement is due to the improved Mn2+ doping efficiency and the effective passivation of native vacancy defects. The stability of the NCs is enhanced by replacing Pb2+ with Mg2+ and Mn2+, mitigating lattice distortions within the [PbCl6]4− octahedral framework. The color rendering index of white light‐emitting diodes fabricated with the post‐treated Mn2+:CsPbCl3 NCs achieves an exceptional value of 98. This work offers novel insights into the fabrication of high‐PLQY Mn2+:CsPbCl3 NCs, advancing the practical deployment of perovskite nanomaterials in various industries.
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