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Crystallographic, Optical, and Electronic Properties of the Cs2AgBi1–xInxBr6 Double Perovskite: Understanding the Fundamental Photovoltaic Efficiency Challenges

  • Laura Schade
    Laura Schade
    Clarendon Laboratory, Department of Physics, University of Oxford, Oxford OX1 3 PU, United Kingdom
    More by Laura Schade
  • Suhas Mahesh
    Suhas Mahesh
    Clarendon Laboratory, Department of Physics, University of Oxford, Oxford OX1 3 PU, United Kingdom
    More by Suhas Mahesh
  • George Volonakis
    George Volonakis
    Université Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes), UMR 6226, Rennes, France
  • Marios Zacharias
    Marios Zacharias
    Department of Mechanical and Materials Science Engineering, Cyprus University of Technology, P.O. Box 50329, 3603 Limassol, Cyprus
  • Bernard Wenger
    Bernard Wenger
    Clarendon Laboratory, Department of Physics, University of Oxford, Oxford OX1 3 PU, United Kingdom
  • Felix Schmidt
    Felix Schmidt
    School of Life Sciences, Institute for Ecopreneurship, University of Applied Sciences and Arts Northwestern Switzerland (FHNW), 4132 Muttenz, Switzerland
  • Sameer Vajjala Kesava
    Sameer Vajjala Kesava
    Clarendon Laboratory, Department of Physics, University of Oxford, Oxford OX1 3 PU, United Kingdom
  • Dharmalingam Prabhakaran
    Dharmalingam Prabhakaran
    Clarendon Laboratory, Department of Physics, University of Oxford, Oxford OX1 3 PU, United Kingdom
  • Mojtaba Abdi-Jalebi
    Mojtaba Abdi-Jalebi
    Institute for Materials Discovery, University College London, Malet Place, London WC1E 7JE, United Kingdom
    Cavendish Laboratory, Department of Physics, University of Cambridge, JJ Thomson Avenue, Cambridge CB3 0HE, United Kingdom
  • Markus Lenz
    Markus Lenz
    School of Life Sciences, Institute for Ecopreneurship, University of Applied Sciences and Arts Northwestern Switzerland (FHNW), 4132 Muttenz, Switzerland
    More by Markus Lenz
  • Feliciano Giustino
    Feliciano Giustino
    Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin, Austin, Texas 78712, United States
    Department of Physics, The University of Texas at Austin, Austin, Texas 78712, United States
  • Giulia Longo
    Giulia Longo
    Department of Mathematics, Physics and Electrical Engineering, Northumbria University, Ellison Place, Newcastle upon Tyne NE18ST, United Kingdom
    More by Giulia Longo
  • Paolo G. Radaelli
    Paolo G. Radaelli
    Clarendon Laboratory, Department of Physics, University of Oxford, Oxford OX1 3 PU, United Kingdom
  • , and 
  • Henry J. Snaith*
    Henry J. Snaith
    Clarendon Laboratory, Department of Physics, University of Oxford, Oxford OX1 3 PU, United Kingdom
    *[email protected]
Cite this: ACS Energy Lett. 2021, 6, 3, 1073–1081
Publication Date (Web):February 19, 2021
https://doi.org/10.1021/acsenergylett.0c02524
Copyright © 2021 American Chemical Society

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    Abstract

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    We present a crystallographic and optoelectronic study of the double perovskite Cs2AgBi1–xInxBr6. From structural characterization we determine that the indium cation shrinks the lattice and shifts the cubic-to-tetragonal phase transition point to lower temperatures. The absorption onset is shifted to shorter wavelengths upon increasing the indium content, leading to wider band gaps, which we rationalize through first-principles band structure calculations. Despite the unfavorable band gap shift, we observe an enhancement in the steady-state photoluminescence intensity, and n-i-p photovoltaic devices present short-circuit current greater than that of neat Cs2AgBiBr6 devices. In order to evaluate the prospects of this material as a solar absorber, we combine accurate absorption measurements with thermodynamic modeling and identify the fundamental limitations of this system. Provided radiative efficiency can be increased and the choice of charge extraction layers are specifically improved, this material could prove to be a useful wide band gap solar absorber.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.0c02524.

    • Indium percentage determined by ICP-MS and XRD in single crystals (TS1) and powders (TS4); plot of F2calc versus F2obs for the structural refinement of Cs2AgInxBi1–xBr6 single crystals (Figure S1) and structural information (Table ST2); Rietveld refinements for Cs2AgInxBi1–xBr6 powders (Figure S2) and related structural information (Table ST3); thin film thickness (Table ST5); thin-film XRD patterns (Figure S3); structural transitions in single crystals (Figures S4–S6); absorption and PL from polycrystalline powders (Figure S7) and photos of samples (Figure S8); optical constants n and k from ellipsometry measurements (Figure S9); computational methods (section 4); PDS and Tauc-plot (Figure S11); band gaps and Urbach energies extrapolated from fittings (Table ST6 and Figure S12); device preparation and characterization in section 6: JV curves (Figure S13), EQE (Figure S14), PCE, and VOC (Figure S15) (PDF)

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    Cited By

    This article is cited by 20 publications.

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