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Magnetic Effect of Dopants on Bright and Dark Excitons in Strongly Confined Mn-Doped CsPbI3 Quantum Dots

  • Tian Qiao
    Tian Qiao
    Department of Chemistry, Texas A&M University, College Station, Texas 777843, United States
    More by Tian Qiao
  • Xiaohan Liu
    Xiaohan Liu
    Department of Physics, Texas A&M University, College Station, Texas 777843, United States
    More by Xiaohan Liu
  • Daniel Rossi
    Daniel Rossi
    Center for Nanomedicine, Institute for Basic Science and Graduate Program of Nano Biomedical Engineering, Advanced Science Institute, Yonsei University, Seoul 03722, Republic of Korea
    More by Daniel Rossi
  • Mohit Khurana
    Mohit Khurana
    Department of Physics, Texas A&M University, College Station, Texas 777843, United States
  • Yulin Lin
    Yulin Lin
    Center for Nanoscale Materials, Argonne National Laboratory, Argonne, Illinois 60439, United States
    More by Yulin Lin
  • Jianguo Wen
    Jianguo Wen
    Center for Nanoscale Materials, Argonne National Laboratory, Argonne, Illinois 60439, United States
    More by Jianguo Wen
  • Jinwoo Cheon
    Jinwoo Cheon
    Center for Nanomedicine, Institute for Basic Science and Graduate Program of Nano Biomedical Engineering, Advanced Science Institute, Yonsei University, Seoul 03722, Republic of Korea
    More by Jinwoo Cheon
  • Alexey V. Akimov
    Alexey V. Akimov
    Department of Physics, Texas A&M University, College Station, Texas 777843, United States
  • , and 
  • Dong Hee Son*
    Dong Hee Son
    Department of Chemistry, Texas A&M University, College Station, Texas 777843, United States
    Center for Nanomedicine, Institute for Basic Science and Graduate Program of Nano Biomedical Engineering, Advanced Science Institute, Yonsei University, Seoul 03722, Republic of Korea
    *Email: [email protected]
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Cite this: Nano Lett. 2021, 21, 22, 9543–9550
Publication Date (Web):November 11, 2021
https://doi.org/10.1021/acs.nanolett.1c03114
Copyright © 2021 American Chemical Society

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    Abstract

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    We investigated the magnetic effect of Mn2+ ions on an exciton of Mn-doped CsPbI3 quantum dots (QDs), where we looked for the signatures of an exciton magnetic polaron known to produce a large effective magnetic field in Mn-doped CdSe QDs. In contrast to Mn-doped CdSe QDs that can produce ∼100 T of magnetic field upon photoexcitation, manifested as a large change in the energy and relaxation dynamics of a bright exciton, Mn-doped CsPbI3 QDs exhibited little influence of a magnetic dopant on the behavior of a bright exciton. However, a μs-lived dark exciton in CsPbI3 QDs showed 40% faster decay in the presence of Mn2+, equivalent to the effect of ∼3 T of an external magnetic field. While further study is necessary to fully understand the origin of the large difference in the magneto-optic property of an exciton in two systems, we consider that the difference in antiferromagnetic coupling of the dopants is an important contributing factor.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.1c03114.

    • Details of the synthesis, time-resolved and static PL at varying temperature and magnetic field, SQUID, EPR, TEM and absorption cross section measurements, additional temperature-dependent PL spectra, comparison of 0.5% and 3.0% Mn-doped CsPbI3 QD data (PDF)

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    Cited By

    This article is cited by 8 publications.

    1. Andries van Hattem, Jean-Christophe Griveau, Eric Colineau, Anton J. E. Lefering, Rudy J. M. Konings, Anna L. Smith. Low-Temperature Heat Capacity of CsPbI3, Cs4PbI6, and Cs3Bi2I9. The Journal of Physical Chemistry C 2023, 127 (46) , 22808-22816. https://doi.org/10.1021/acs.jpcc.3c05846
    2. Avik Das, Tushar Debnath. Giant Exciton Stokes Shift in Interfacially Prepared Cs(Mn/Pb)Cl3 Alloy Nanoplatelets. The Journal of Physical Chemistry Letters 2023, 14 (25) , 5940-5948. https://doi.org/10.1021/acs.jpclett.3c01093
    3. Daniel Weinberg, Yoonjae Park, David T. Limmer, Eran Rabani. Size-Dependent Lattice Symmetry Breaking Determines the Exciton Fine Structure of Perovskite Nanocrystals. Nano Letters 2023, 23 (11) , 4997-5003. https://doi.org/10.1021/acs.nanolett.3c00861
    4. Virendra Kumar, Harish Chandr Chauhan, Vandana Nagal, Aurangzeb Khurram Hafiz, Kedar Singh. Lattice-Distortion-Induced Change in the Magnetic Properties in Br-Defect Host CsPbBr3 Perovskite Quantum Dots. The Journal of Physical Chemistry Letters 2023, 14 (4) , 888-896. https://doi.org/10.1021/acs.jpclett.2c03576
    5. Hyejin Choe, Ho Jin, Seon Joo Lee, Junsang Cho. Exciton Recombination versus Energy Transfer: Mapping Competing Excited-State Dynamics in Various Mn-Doped CsPb(Cl1–yBry)3 Perovskite Nanocrystals for Achieving White Light Emission. ACS Applied Nano Materials 2022, 5 (12) , 18385-18395. https://doi.org/10.1021/acsanm.2c04208
    6. Shuli Wang, Mateusz Dyksik, Carola Lampe, Moritz Gramlich, Duncan K. Maude, Michał Baranowski, Alexander S. Urban, Paulina Plochocka, Alessandro Surrente. Thickness-Dependent Dark-Bright Exciton Splitting and Phonon Bottleneck in CsPbBr3-Based Nanoplatelets Revealed via Magneto-Optical Spectroscopy. Nano Letters 2022, 22 (17) , 7011-7019. https://doi.org/10.1021/acs.nanolett.2c01826
    7. Linzhong Wu, Yiou Wang, Mariam Kurashvili, Amrita Dey, Muhan Cao, Markus Döblinger, Qiao Zhang, Jochen Feldmann, He Huang, Tushar Debnath. Interfacial Manganese‐Doping in CsPbBr 3 Nanoplatelets by Employing a Molecular Shuttle. Angewandte Chemie 2022, 134 (15) https://doi.org/10.1002/ange.202115852
    8. Linzhong Wu, Yiou Wang, Mariam Kurashvili, Amrita Dey, Muhan Cao, Markus Döblinger, Qiao Zhang, Jochen Feldmann, He Huang, Tushar Debnath. Interfacial Manganese‐Doping in CsPbBr 3 Nanoplatelets by Employing a Molecular Shuttle. Angewandte Chemie International Edition 2022, 61 (15) https://doi.org/10.1002/anie.202115852

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