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    CsMnBr3: Lead-Free Nanocrystals with High Photoluminescence Quantum Yield and Picosecond Radiative Lifetime

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    Embargo End Date:
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    Type
    Article
    Authors
    Almutlaq, Jawaher cc
    Mir, Wasim Jeelani cc
    Gutierrez Arzaluz, Luis cc
    Yin, Jun cc
    Vasylevskyi, Serhii
    Maity, Partha cc
    Liu, Jiakai cc
    Naphade, Rounak cc
    Mohammed, Omar F. cc
    Bakr, Osman cc
    KAUST Department
    Material Science and Engineering Program
    Physical Science and Engineering (PSE) Division
    KAUST Solar Center (KSC)
    Physical Characterization
    KAUST Catalysis Center (KCC)
    Chemical Science Program
    Biological and Environmental Sciences and Engineering (BESE) Division
    Date
    2021-02-15
    Embargo End Date
    2022-02-15
    Submitted Date
    2020-12-22
    Permanent link to this record
    http://hdl.handle.net/10754/667481
    
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    Abstract
    Lead halide compounds, including lead halide perovskite nanocrystals (NCs), have attracted the interest of researchers in optoelectronics and photonics because of their high photoluminescence quantum yields (PLQYs) coupled with relatively short PL lifetimes (on the order of a few nanoseconds). However, lead-free metal halides of high PLQY, including double perovskites and their doped NCs, typically possess long PL lifetimes (up to microseconds) that limit their application space. Here, we introduce CsMnBr3 NCs, which are lead-free and red-emitting, that combine a high PLQY with an exceptionally short radiative lifetime (on the order of picoseconds). We find that the octahedral coordination of Mn2+ in CsMnBr3 induces a red emission centered at ∼643 nm with a PLQY of ∼54% and a fast radiative decay rate. Femtosecond transient absorption and transient PL spectroscopies reveal the existence of a low-lying excited state of Mn2+ that relaxes to the ground state within around 605 ps by emitting light at around 643 nm. At greater excitation energies, higher excited states of Mn2+ relax in the sub-nanosecond time scale to this low-lying excited state. A similarly positioned PL peak with a short picosecond scale PL lifetime and a PLQY of ∼6.7% was also detected in bulk CsMnBr3 single crystals reported in this study—a relatively high quantum yield for a bulk material. Our experimental results and density functional theory modelling show that the crystal structure and the strong coupling among Mn2+ ions govern those luminescence properties of CsMnBr3 NCs and single crystals. These findings pave the way for new lead-free materials that combine high PLQY and ultrafast luminescence.
    Citation
    Almutlaq, J., Mir, W. J., Gutiérrez-Arzaluz, L., Yin, J., Vasylevskyi, S., Maity, P., … Bakr, O. M. (2021). CsMnBr3: Lead-Free Nanocrystals with High Photoluminescence Quantum Yield and Picosecond Radiative Lifetime. ACS Materials Letters, 290–297. doi:10.1021/acsmaterialslett.0c00603
    Publisher
    American Chemical Society (ACS)
    Journal
    ACS Materials Letters
    DOI
    10.1021/acsmaterialslett.0c00603
    Additional Links
    https://pubs.acs.org/doi/10.1021/acsmaterialslett.0c00603
    ae974a485f413a2113503eed53cd6c53
    10.1021/acsmaterialslett.0c00603
    Scopus Count
    Collections
    Articles; Biological and Environmental Sciences and Engineering (BESE) Division; Physical Science and Engineering (PSE) Division; Chemical Science Program; Material Science and Engineering Program; KAUST Catalysis Center (KCC); KAUST Solar Center (KSC)

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