Nanoscale interfacial engineering enables highly stable and efficient perovskite photovoltaics
Anurag Krishna a, Hong Zhang b, Zhiwen Zhou b, Thibaut Gallet c, Mathias Dankl d, Olivier Ouellette b, Felix Eickemeyer b, Fan Fu e, Mounir Mensi f, Shaik M. Zakeeruddin b, Ursula Roethlisberger d, G. N. Manjunatha Reddy g, Alex Redinger c, Michael Graetzel b, Anders Hagfeldt a h
a Laboratory of Photomolecular Science, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, Switzerland
b Laboratory of Photonics and Interfaces, École Polytechnique Fédérale de Lausanne, Switzerland
c Scanning Probe Microscopy Laboratory, Department of Physics and Materials Science, University of Luxembourg, Luxembourg
d Laboratory of Computational Chemistry and Biochemistry, École Polytechnique Fédérale de Lausanne, Switzerland
e Laboratory for Thin Films and Photovoltaics, Empa-Swiss Federal Laboratories for Materials Science and Technology, Switzerland.
f Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, Valais Wallis, Sion, Switzerland.
g Univ. Lille, CNRS, Centrale Lille Institut, Univ. Artois, UMR 8181-UCCS-Unité de Catalyse et Chimie du Solide, F-59000 Lille, France
h Department of Chemistry – Ångström Laboratory, Uppsala University, Sweden
International Conference on Hybrid and Organic Photovoltaics
Proceedings of 13th Conference on Hybrid and Organic Photovoltaics (HOPV21)
Online, Spain, 2021 May 24th - 28th
Organizers: Marina Freitag, Feng Gao and Sam Stranks
Oral, Anurag Krishna, presentation 005
Publication date: 11th May 2021

Long-term operational stability remains the primary concern for perovskite solar cells. Consequently, there is a quest for searching for new compositions that enable stable and efficient perovskites. We report a new molecular-level interface engineering strategy using a multifunctional ligand that augments long-term operational and thermal stability by chemically modifying the formamidinium lead iodide rich photoactive layer. The surface derivatized solar cells exhibited high operational stability (maximum powering point tracking at 1 sun) with a stabilized T80 (the time over which the device efficiency reduces to 80% of its initial value of post-burn-in) of ≈5950 h at 40 ºC and stabilized efficiency over 23%. The origin of high device stability and performance is correlated to the nano/sub-nanoscale molecular level interactions between ligand and perovskite layer, which is corroborated by comprehensive multiscale characterization. Our results provide key insights into the modulation of the grain boundaries, local density of states, surface bandgap, and interfacial recombination. Chemical analysis of the aged devices showed that interface passivation inhibited ion migration and prevented photoinduced I2 release that irreversibly degrades the perovskite. This study shows that passivating ligands have the potential to overcome stability issues associated with the high performing hybrid perovskite compositions, thus allowing a step closer to achieving long-standing stability of perovskite-based solar cells.

This project has received funding from the European Union’s Horizon 2020 Research and Innovation program under the Marie Skłodowska-Curie Grant Agreement No. 843453. H.Z., S.M.Z., and M. G. acknowledge the funding from the European Union’s Horizon 2020 research and innovation program GRAPHENE Flagship Core 3 grant agreement No.: 881603. A. K. and A. H. acknowledge EUSMI Grant No. E200900442 for access to 800 MHz spectrometer to conduct solid-state NMR measurements. G.N.M.R acknowledges financial support from University of Lille and IR-RMN-THC FR-3050 CNRS France. T.G. and A.R. acknowledge funding from the Fonds National de la Recherche Luxembourg under the project “Sunspot” No 11244141. F.F. acknowledges funding from the Swiss Federal Office of Energy (SFOE)-BFE (project no. SI/501805-01). O.O. acknowledges funding from the National Sciences and Engineering Research Council of Canada. U.R. acknowledges Swiss National Science Foundation Grant No. 200020-165863 and the NCCR-MUST for funding as well as computational resources from the Swiss National Computing Centre CSCS. The authors acknowledge the help of Dr. Sandy Sanchez and Dr. Wen Hua Bi for the assistance in SEM and GIXRD measurements, respectively.

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