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Unveiling the Excited-State Dynamics of Mn2+ in 0D Cs4PbCl6 Perovskite Nanocrystals
Wen Zhang1,2, Jiaojiao Wei1, Zhongliang Gong1
1CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences Fuzhou Fujian 350002 China.
Abstract:
Doping is an effective strategy for tailoring the optical properties of 0D Cs4PbX6 (X = Cl, Br, and I) perovskite nanocrystals (NCs) and expanding their applications. Herein, a unique approach is reported for the controlled synthesis of pure-phase Mn2+-doped Cs4PbCl6 perovskite NCs and the excited-state dynamics of Mn2+ is unveiled through temperature-dependent steady-state and transient photoluminescence (PL) spectroscopy. Because of the spatially confined 0D structure of Cs4PbCl6 perovskite, the NCs exhibit drastically different PL properties of Mn2+ in comparison with their 3D CsPbCl3 analogues, including significantly improved PL quantum yield in solid form (25.8%), unusually long PL lifetime (26.2 ms), large exciton binding energy, strong electron-phonon coupling strength, and an anomalous temperature evolution of Mn2+-PL decay from a dominant slow decay (in tens of ms scale) at 300 K to a fast decay (in 1 ms scale) at 10 K. These findings provide fundamental insights into the excited-state dynamics of Mn2+ in 0D Cs4PbCl6 NCs, thus laying a foundation for future design of 0D perovskite NCs through metal ion doping toward versatile applications.
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