Title
Nano-emitting Heterostructures Violate Optical Reciprocity and Enable Efficient Photoluminescence in Halide-Segregated Methylammonium-Free Wide Bandgap Perovskites
Date Issued
12 February 2021
Access level
metadata only access
Resource Type
journal article
Author(s)
Caprioglio P.
Caicedo-Dávila S.
Yang T.C.J.
Wolff C.M.
Peña-Camargo F.
Fiala P.
Ballif C.
Abou-Ras D.
Stolterfoht M.
Albrecht S.
Jeangros Q.
Neher D.
Institute for Silicon Photovoltaics
Publisher(s)
American Chemical Society
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.
Start page
419
End page
428
Volume
6
Issue
2
Language
English
OCDE Knowledge area
Ingeniería de materiales
Scopus EID
2-s2.0-85099647124
Source
ACS Energy Letters
ISSN of the container
23808195
Sponsor(s)
We acknowledge HyPerCells (a joint graduate school of the University of Potsdam and the Helmholtz-Zentrum Berlin) and the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) - project number 423749265 and 424709669 - SPP 2196 (SURPRISE and HIPSTER) for funding. We also acknowledge financial support by the Federal Ministry for Economic Affairs and Energy within the framework of the 7th Energy Research Programme (P3T-HOPE, 03EE1017C). S.C.D. and D.A.R. are grateful for the financial support by the Helmholtz International Research School HI-SCORE (HIRS- 0008) and by the HyPerCells Graduate School. C.B., Q.J., and P.F. would like to acknowledge the Swiss Federal Office of Energy (SI/501804-01 INTENT) and the Swiss National Science Foundation (176552 Bridge Power and CRSII5_171000 Sinergia Episode). T.C.-J.Y. would like to acknowledge the support of the EU Horizon 2020 Marie Skłodowska-Curie Individual Fellowship under grant “POSITS”, No. 747221. T.C.-J.Y would like to acknowledge the support of a Marie Skłodowska-Curie Individual Fellowship from the European Union’s Horizon 2020 Research and Innovation Program (Grant Agreement No. 747221, action acronym: POSITS). T.C.-J.Y. would like to thank the CSIRO Research Office for project funding and Fellowship support. Bundesamt für Energie - SI/501804-01 INTENT - UFE Helmholtz-Zentrum für Umweltforschung - UFZ Bundesministerium für Wirtschaft und Energie - 03EE1017C - BMWi Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung - CRSII5_171000, 176552 - SNF Horizon 2020 Framework Programme - H2020
Sources of information: Directorio de Producción Científica Scopus