journal article·2018-08-28

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

Julian A. Steele, Pascal Puech, Masoumeh Keshavarz, Ruoxi Yang, Subhasree Banerjee, Elke Debroye, Cheol Woong Kim, Haifeng Yuan, Nam Ho Heo, Johan Vanacken, Aron Walsh, Johan Hofkens, Maarten B. J. Roeffaers

ACS Nano· Volume 12· Issue 8
Publisher page

Abstract

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 Cs2AgBiBr6 via 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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Research context

OpenAlex topics: Perovskite Materials and Applications · Solid-state spectroscopy and crystallography · Optical properties and cooling technologies in crystalline materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Centre for Surface Chemistry and Catalysis, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium

CEMES/CNRS, Université de Toulouse, 29, rue Jeanne Marvig, 31055 Toulouse, France

Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium

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

School of Science, Department of Chemistry, Adamas University, Barasat-Barrackpore Road, Kolkata 700126, West Bengal, India

Department of Applied Chemistry, School of Applied Chemical Engineering, College of Engineering, Kyungpook National University, Daegu 41566, Korea

INPAC-Institute for Nanoscale Physics and Chemistry, KU Leuven, Celestijnenlaan 200 D, B-3001 Leuven, Belgium

Global E3 Institute and Department of Materials Science and Engineering, Yonsei University, Seoul 120-749, Korea

Funding

KU Leuven · Federaal Wetenschapsbeleid · Fonds Wetenschappelijk Onderzoek · FP7 Ideas: European Research Council · Hercules foundation · Flemish Government

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