journal article·2021-02-12Open access

Nano-emitting Heterostructures Violate Optical Reciprocity and Enable Efficient Photoluminescence in Halide-Segregated Methylammonium-Free Wide Bandgap Perovskites

Pietro Caprioglio, Sebastián Caicedo-Dávila, Terry Chien-Jen Yang, Christian M. Wolff, Francisco Peña-Camargo, Peter Fiala, Bernd Rech, Christophe Ballif, Daniel Abou-Ras, Martin Stolterfoht, Steve Albrecht, Quentin Jeangros, Dieter Neher

ACS Energy Letters· Volume 6· Issue 2

Abstract

This work investigates halide segregation in methylammonium-free wide bandgap perovskites by photoluminescence quantum yield (PLQY) and advanced electron microscopy techniques. Our study reveals how the formation of nano-emitting low-energy domains embedded in a wide bandgap matrix, located at surfaces and grain boundaries, enables a PLQY up to 25%. Intensity-dependent PLQY measurement and PL excitation spectroscopy revealed efficient charge funnelling and the failure of optical reciprocity between absorption and emission, limiting the use of PLQY data to determine the quasi-Fermi level splitting (QFLS) in these layers. Concomitantly, the small spectral overlap between emission and absorption reduces photon re-absorption. We demonstrate that phase segregation and charge funnelling, although harmful for the radiative efficiency of the mixed phase, are essential for achieving high PLQYs, selectively at low energies, otherwise not achievable in non-segregated perovskites with a similar bandgap. This promotes the applicability of this phenomenon in thermally stable high-efficiency emitting devices and color-conversion heterostructures.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Perovskite Materials and Applications · Quantum Dots Synthesis And Properties · Chalcogenide Semiconductor Thin Films

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

Affiliations

Institute of Physics and Astronomy, University of Potsdam, 14476 Potsdam, Germany

Young Investigator Group Perovskite Tandem Solar Cells, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, 12489 Berlin, Germany

Clarendon Laboratory, Department of Physics, University of Oxford, Oxford OX1 3PU, United Kingdom

Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, 12489 Berlin, Germany

Institute of Microengineering (IMT), Photovoltaics and Thin-Film Electronics Laboratory (PV-Lab), École Polytechnique Fédérale de Lausanne (EPFL), Rue de la Maladière 71b, 2002 Neuchâtel, Switzerland

CSIRO Energy Centre, 10 Murray Dwyer Circuit, Mayfield West, NSW 2304, Australia

Institute for Silicon Photovoltaics, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, 12489 Berlin, Germany

Faculty IV − Electrical Engineering and Computer Science, Technical University Berlin, 10587 Berlin, Germany

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