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Giant Electron–Phonon Coupling and Deep Conduction Band Resonance in Metal Halide Double Perovskite

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    Giant Electron–Phonon Coupling and Deep Conduction Band Resonance in Metal Halide Double Perovskite
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    • Julian A. Steele*
      Julian A. Steele
      Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium
      *E-mail: [email protected]
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      Orcidhttp://orcid.org/0000-0001-7982-4413
    • Pascal Puech
      Pascal Puech
      CEMES/CNRS, Université de Toulouse, 29, rue Jeanne Marvig, 31055 Toulouse, France
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    • Masoumeh Keshavarz
      Masoumeh Keshavarz
      Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium
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      Orcidhttp://orcid.org/0000-0003-3685-6778
    • Ruoxi Yang
      Ruoxi Yang
      Department of Materials, Imperial College London, Exhibition Road, London SW7 2AZ, United Kingdom
      Department of Chemistry, University of Bath, Claverton Down, Bath BA2 7AY, United Kingdom
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    • Subhasree Banerjee
      Subhasree Banerjee
      Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium
      School of Science, Department of Chemistry, Adamas University, Barasat-Barrackpore Road, Kolkata 700126, West Bengal, India
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    • Elke Debroye
      Elke Debroye
      Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium
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    • Cheol Woong Kim
      Cheol Woong Kim
      Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium
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      Orcidhttp://orcid.org/0000-0002-7053-9744
    • Haifeng Yuan
      Haifeng Yuan
      Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium
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      Orcidhttp://orcid.org/0000-0001-6652-3670
    • Nam Ho Heo
      Nam Ho Heo
      Department of Applied Chemistry, School of Applied Chemical Engineering, College of Engineering, Kyungpook National University, Daegu 41566, Korea
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      Orcidhttp://orcid.org/0000-0003-4689-0080
    • Johan Vanacken
      Johan Vanacken
      INPAC-Institute for Nanoscale Physics and Chemistry, KU Leuven, Celestijnenlaan 200 D, B-3001 Leuven, Belgium
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    • Aron Walsh
      Aron Walsh
      Department of Materials, Imperial College London, Exhibition Road, London SW7 2AZ, United Kingdom
      Global E3 Institute and Department of Materials Science and Engineering, Yonsei University, Seoul 120-749, Korea
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      Orcidhttp://orcid.org/0000-0001-5460-7033
    • Johan Hofkens
      Johan Hofkens
      Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium
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      Orcidhttp://orcid.org/0000-0002-9101-0567
    • Maarten B. J. Roeffaers
      Maarten B. J. Roeffaers
      Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium
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    ACS Nano

    Cite this: ACS Nano 2018, 12, 8, 8081–8090
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    https://doi.org/10.1021/acsnano.8b02936
    Published August 7, 2018
    Copyright © 2018 American Chemical Society
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    Abstract

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    The room-temperature charge carrier mobility and excitation–emission properties of metal halide perovskites are governed by their electronic band structures and intrinsic lattice phonon scattering mechanisms. Establishing how charge carriers interact within this scenario will have far-reaching consequences for developing high-efficiency materials for optoelectronic applications. Herein we evaluate the charge carrier scattering properties and conduction band environment of the double perovskite Cs2AgBiBr6via a combinatorial approach; single crystal X-ray diffraction, optical excitation and temperature-dependent emission spectroscopy, resonant and nonresonant Raman scattering, further supported by first-principles calculations. We identify deep conduction band energy levels and that scattering from longitudinal optical phonons—via the Fröhlich interaction—dominates electron scattering at room temperature, manifesting within the nominally nonresonant Raman spectrum as multiphonon processes up to the fourth order. A Fröhlich coupling constant nearing 230 meV is inferred from a temperature-dependent emission line width analysis and is found to be extremely large compared to popular lead halide perovskites (between 40 and 60 meV), highlighting the fundamentally different nature of the two “single” and “double” perovskite materials branches.

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.8b02936.

    • Crystallographic information derived from single crystal XRD, group factor analysis and Cs2AgBiBr6 vibrational assignment, EDX and Raman spectroscopic mapping of the so-called yellow phase, power dependence of laser-induced Cs2AgBiBr6 surface modifications, low-temperature Raman spectrum, and a comparison of the temperature dependence of Cs2AgBiBr6 emission line width before and after thermal annealing (PDF)

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    Cited By

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    This article is cited by 211 publications.

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