Unveiling the Excited‐State Dynamics of Mn2+ in 0D Cs4PbCl6 Perovskite Nanocrystals

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...

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Main Authors: Wen Zhang, Jiaojiao Wei, Zhongliang Gong, Ping Huang, Jin Xu, Renfu Li, Shaohua Yu, Xingwen Cheng, Wei Zheng, Xueyuan Chen
Format: Article
Language:English
Published: Wiley 2020-11-01
Series:Advanced Science
Subjects:
Online Access:https://doi.org/10.1002/advs.202002210
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author Wen Zhang
Jiaojiao Wei
Zhongliang Gong
Ping Huang
Jin Xu
Renfu Li
Shaohua Yu
Xingwen Cheng
Wei Zheng
Xueyuan Chen
author_facet Wen Zhang
Jiaojiao Wei
Zhongliang Gong
Ping Huang
Jin Xu
Renfu Li
Shaohua Yu
Xingwen Cheng
Wei Zheng
Xueyuan Chen
author_sort Wen Zhang
collection DOAJ
description 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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spelling doaj.art-5c06e18a6a8248a7838905495b16823d2022-12-22T00:56:28ZengWileyAdvanced Science2198-38442020-11-01722n/an/a10.1002/advs.202002210Unveiling the Excited‐State Dynamics of Mn2+ in 0D Cs4PbCl6 Perovskite NanocrystalsWen Zhang0Jiaojiao Wei1Zhongliang Gong2Ping Huang3Jin Xu4Renfu Li5Shaohua Yu6Xingwen Cheng7Wei Zheng8Xueyuan Chen9CAS 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 ChinaCAS 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 ChinaCAS 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 ChinaCAS 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 ChinaCAS 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 ChinaCAS 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 ChinaCAS 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 ChinaCAS 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 ChinaCAS 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 ChinaCAS 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 ChinaAbstract 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.https://doi.org/10.1002/advs.202002210energy transferexcited‐state dynamicsmanganeseperovskite nanocrystalsphotoluminescence
spellingShingle Wen Zhang
Jiaojiao Wei
Zhongliang Gong
Ping Huang
Jin Xu
Renfu Li
Shaohua Yu
Xingwen Cheng
Wei Zheng
Xueyuan Chen
Unveiling the Excited‐State Dynamics of Mn2+ in 0D Cs4PbCl6 Perovskite Nanocrystals
Advanced Science
energy transfer
excited‐state dynamics
manganese
perovskite nanocrystals
photoluminescence
title Unveiling the Excited‐State Dynamics of Mn2+ in 0D Cs4PbCl6 Perovskite Nanocrystals
title_full Unveiling the Excited‐State Dynamics of Mn2+ in 0D Cs4PbCl6 Perovskite Nanocrystals
title_fullStr Unveiling the Excited‐State Dynamics of Mn2+ in 0D Cs4PbCl6 Perovskite Nanocrystals
title_full_unstemmed Unveiling the Excited‐State Dynamics of Mn2+ in 0D Cs4PbCl6 Perovskite Nanocrystals
title_short Unveiling the Excited‐State Dynamics of Mn2+ in 0D Cs4PbCl6 Perovskite Nanocrystals
title_sort unveiling the excited state dynamics of mn2 in 0d cs4pbcl6 perovskite nanocrystals
topic energy transfer
excited‐state dynamics
manganese
perovskite nanocrystals
photoluminescence
url https://doi.org/10.1002/advs.202002210
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