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Nanoscale heterogeneity of ultrafast many-body carrier dynamics in triple cation perovskites

Author

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  • Jun Nishida

    (University of Colorado
    JILA, University of Colorado)

  • Peter T. S. Chang

    (University of Colorado
    JILA, University of Colorado)

  • Jiselle Y. Ye

    (University of Colorado)

  • Prachi Sharma

    (University of Colorado)

  • Dylan M. Wharton

    (University of Colorado
    JILA, University of Colorado)

  • Samuel C. Johnson

    (University of Colorado
    JILA, University of Colorado)

  • Sean E. Shaheen

    (University of Colorado
    University of Colorado
    Renewable and Sustainable Energy Institute, University of Colorado)

  • Markus B. Raschke

    (University of Colorado
    JILA, University of Colorado)

Abstract

In high fluence applications of lead halide perovskites for light-emitting diodes and lasers, multi-polaron interactions and associated Auger recombination limit the device performance. However, the relationship of the ultrafast and strongly lattice coupled carrier dynamics to nanoscale heterogeneities has remained elusive. Here, in ultrafast visible-pump infrared-probe nano-imaging of the photoinduced carrier dynamics in triple cation perovskite films, a ~20 % variation in sub-ns relaxation dynamics with spatial disorder on tens to hundreds of nanometer is resolved. We attribute the non-uniform relaxation dynamics to the heterogeneous evolution of polaron delocalization and increasing scattering time. The initial high-density excitation results in faster relaxation due to strong many-body interactions, followed by extended carrier lifetimes at lower densities. These results point towards the missing link between the optoelectronic heterogeneity and associated carrier dynamics to guide synthesis and device engineering for improved perovskites device performance.

Suggested Citation

  • Jun Nishida & Peter T. S. Chang & Jiselle Y. Ye & Prachi Sharma & Dylan M. Wharton & Samuel C. Johnson & Sean E. Shaheen & Markus B. Raschke, 2022. "Nanoscale heterogeneity of ultrafast many-body carrier dynamics in triple cation perovskites," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33935-0
    DOI: 10.1038/s41467-022-33935-0
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    References listed on IDEAS

    as
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