journal article·2021-06-22Open access

Large Cation Engineering in Two-Dimensional Silver–Bismuth Bromide Double Perovskites

Fabian Schmitz, Jonas Horn, Nicola Dengo, Alexander E. Sedykh, Jonathan Becker, Elena Maiworm, Péter Bélteky, Ákos Kukovecz, Silvia Gross, Francesco Lamberti, Klaus Müller-Buschbaum, Derck Schlettwein, Daniele Meggiolaro, Marcello Righetto, Teresa Gatti

Chemistry of Materials· Volume 33· Issue 12

Abstract

Double perovskites are promising candidates for less toxic and highly stable metal halide perovskites, but their optoelectronic performances still lag behind those of the lead halide counterpart, due to the indirect nature of the bandgap and the strong electron–phonon coupling. Reducing the dimensionality of Cs2AgBiBr6 down to a 2D layered form is strategic in order to tune the band gap from indirect to direct and provides new insights into the structure–property relationships of double perovskites. Herein, we report on a series of monolayer 2D hybrid double perovskites of formula (RA)4AgBiBr8, where RA represents different primary ammonium large cations with alkyl- and aryl-based functionalities. An in-depth experimental characterization of structure, film morphology, and optical properties of these perovskites is carried out. Interestingly, the variation of the ammonium cation and the interplanar distance between adjacent inorganic monolayers has peculiar effects on the film-forming ability and light emission properties of the perovskites. Experiments have been combined with DFT calculations in order to understand the possible origin of the different emissive features. Our study provides a toolbox for future rational developments of 2D double perovskites, with the aim of narrowing the gap with lead halide perovskite optoelectronic properties.
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Research context

OpenAlex topics: Perovskite Materials and Applications · 2D Materials and Applications · Solid-state spectroscopy and crystallography

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

Affiliations

Center for Materials Research, Justus Liebig University, Heinrich Buff Ring 16, 35392 Giessen, Germany

Institute of Physical Chemistry, Justus Liebig University, Heinrich Buff Ring 17, 35392 Giessen, Germany

Institute of Applied Physics, Justus Liebig University, Heinrich Buff Ring 16, 35392 Giessen, Germany

Department of Chemical Sciences, University of Padova, via Marzolo 1, 35131 Padova, Italy

Institute of Inorganic and Analytical Chemistry, Justus Liebig University, Heinrich-Buff-Ring 17, 35392 Giessen, Germany

Interdisciplinary Excellence Centre, Department of Applied and Environmental Chemistry, University of Szeged, Rerrich Béla tér 1, H-6720 Szeged, Hungary

Interdepartmental Centre Giorgio Levi Cases for Energy Economics and Technology, University of Padova, via Marzolo 9, 35131 Padova, Italy

Computational Laboratory for Hybrid/Organic Photovoltaics (CLHYO), Istituto CNR di Scienze e Tecnologie Chimiche “Giulio Natta” (CNR-SCITEC), Via Elce di Sotto 8, 06123 Perugia, Italy

Department of Physics and Astronomy, University College London, London WC1E 6BT, United Kingdom

Funding

Horizon 2020 Framework Programme

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