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Hot Carrier Dynamics in Perovskite Nanocrystal Solids: Role of the Cold Carriers, Nanoconfinement, and the Surface

  • Thomas R. Hopper
    Thomas R. Hopper
    Department of Chemistry, Imperial College London, London W12 0BZ, United Kingdom
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    Orcidhttp://orcid.org/0000-0001-5084-1914
  • , 
  • Andrei Gorodetsky
    Andrei Gorodetsky
    Department of Chemistry, Imperial College London, London W12 0BZ, United Kingdom
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    Orcidhttp://orcid.org/0000-0001-5440-2185
  • , 
  • Ahhyun Jeong
    Ahhyun Jeong
    Department of Chemistry, Imperial College London, London W12 0BZ, United Kingdom
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  • , 
  • Franziska Krieg
    Franziska Krieg
    Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, CH-8093 Zürich, Switzerland
    Laboratory for Thin Films and Photovoltaics, Empa − Swiss Federal Laboratories for Materials Science and Technology, CH-8600 Dübendorf, Switzerland
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    Orcidhttp://orcid.org/0000-0002-0370-1318
  • , 
  • Maryna I. Bodnarchuk
    Maryna I. Bodnarchuk
    Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, CH-8093 Zürich, Switzerland
    Laboratory for Thin Films and Photovoltaics, Empa − Swiss Federal Laboratories for Materials Science and Technology, CH-8600 Dübendorf, Switzerland
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    Orcidhttp://orcid.org/0000-0001-6597-3266
  • , 
  • Marios Maimaris
    Marios Maimaris
    Department of Chemistry, Imperial College London, London W12 0BZ, United Kingdom
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    Orcidhttp://orcid.org/0000-0003-3474-9565
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  • Marine Chaplain
    Marine Chaplain
    Department of Chemistry, Imperial College London, London W12 0BZ, United Kingdom
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  • , 
  • Thomas J. Macdonald
    Thomas J. Macdonald
    Department of Chemistry, Imperial College London, London W12 0BZ, United Kingdom
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    Orcidhttp://orcid.org/0000-0002-7520-6893
  • , 
  • Xiaokun Huang
    Xiaokun Huang
    Institute for High-Frequency Technology, Technische Universität Braunschweig, Schleinitzstrasse 22, 38106 Braunschweig, Germany
    InnovationLab, Speyerer Strasse 4, 69115 Heidelberg, Germany
    Kirchhoff Institute for Physics, University of Heidelberg, 69120 Heidelberg, Germany
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  • , 
  • Robert Lovrincic
    Robert Lovrincic
    Institute for High-Frequency Technology, Technische Universität Braunschweig, Schleinitzstrasse 22, 38106 Braunschweig, Germany
    InnovationLab, Speyerer Strasse 4, 69115 Heidelberg, Germany
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    Orcidhttp://orcid.org/0000-0001-5429-5586
  • , 
  • Maksym V. Kovalenko
    Maksym V. Kovalenko
    Institute of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, CH-8093 Zürich, Switzerland
    Laboratory for Thin Films and Photovoltaics, Empa − Swiss Federal Laboratories for Materials Science and Technology, CH-8600 Dübendorf, Switzerland
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    Orcidhttp://orcid.org/0000-0002-6396-8938
  • , and 
  • Artem A. Bakulin*
    Artem A. Bakulin
    Department of Chemistry, Imperial College London, London W12 0BZ, United Kingdom
    *E-mail: [email protected]
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    Orcidhttp://orcid.org/0000-0002-3998-2000
Cite this: Nano Lett. 2020, 20, 4, 2271–2278
Publication Date (Web):March 6, 2020
https://doi.org/10.1021/acs.nanolett.9b04491
Copyright © 2020 American Chemical Society
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    Abstract

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    Carrier cooling is of widespread interest in the field of semiconductor science. It is linked to carrier–carrier and carrier–phonon coupling and has profound implications for the photovoltaic performance of materials. Recent transient optical studies have shown that a high carrier density in lead-halide perovskites (LHPs) can reduce the cooling rate through a “phonon bottleneck”. However, the role of carrier–carrier interactions, and the material properties that control cooling in LHPs, is still disputed. To address these factors, we utilize ultrafast “pump–push–probe” spectroscopy on LHP nanocrystal (NC) films. We find that the addition of cold carriers to LHP NCs increases the cooling rate, competing with the phonon bottleneck. By comparing different NCs and bulk samples, we deduce that the cooling behavior is intrinsic to the LHP composition and independent of the NC size or surface. This can be contrasted with other colloidal nanomaterials, where confinement and trapping considerably influence the cooling dynamics.

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    • Experimental methods; absorption and PL spectra for the NC films and solutions; electron micrographs for all NC samples; fluence-dependent pump–probe data for NC samples; push fluence-dependent bleach kinetics (PDF)

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