Impact of materials stoichiometry and surface morphology on stability of perovskite solar cells
Roja Singh a b, Hang Hu a b, Thomas Feeney b, Alexander Diercks b, Felix Laufer b, Yang Li a b, The Duong c, Fabian Schackmar a b, Bahram A. Nejand a b, Ulrich W. Paetzold a b
a Institute of Microstructure Technology (IMT), Karlsruhe Institute of Technology (KIT), Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany.
b Light Technology Institute (LTI), Karlsruhe Institute of Technology (KIT), Engesserstrasse 13, 76131 Karlsruhe, Germany.
c School of Engineering, The Australian National University, Canberra 2601, Australia
Oral, Roja Singh, presentation 050
Publication date: 6th February 2024

Long-term stability of perovskite solar cells (PSC) is the impending bottleneck for commercialization of the technology in the renewable energy sector. In this work, we critically assess effects of material stoichiometry and surface morphology to understand their impact on the long-term stability of caesium-formamidinium-based PSC. Key findings demonstrate that the variation in the perovskite precursor - lead iodide (PbI2) to formamidinium iodide (FAI) ratio impacts the stability under various stress conditions (elevated temperature and light). A high molar ratio PbI2/FAI >1.1 in the perovskite precursor contributes to a higher open-circuit voltage (VOC) and hence better power conversion efficiency (PCE). However, the quenching techniques (anti-solvent and vacuum quenching) during the processing do not affect the long-term stability of PSCs. When tested under ISOS-D2 (dark, 85 °C, intermittent current density-voltage J-V characterization) condition, the degradation of the perovskite layer or interfaces between the perovskite layer and the charge transport layers lead to a decrease in performance for the devices implementing non-standard PbI2/FAI ratio (>1.1 or <1.1) over a period of 500 h. Under ISOS-L1 (100 mW/cm2, 25 °C, maximum power point tracking) condition, the devices with PbI2/FAI ≤1.1 remain stable over 500 h whereas devices with PbI2/FAI >1.1 show a drastic drop in J. Interestingly, we observe a contradictory trend in post-degradation analysis of devices stressed under ISOS-L1. The devices with PbI2/FAI ≤1.1 are stable under stress but their PCEs begin to decrease during storage in dark as characterized by intermittent J-V. The presence of iodide vacancies (VI-) in the absorber layer results in non-radiative recombination and migration of iodide ions (I-) to the hole transport layer causes formation of shunts during storage in the dark. This work highlights the importance of reporting stability under different stress conditions as well as post-degradation and dark recovery analysis of PSCs to understand a process as complex as perovskite instability.

Financial support by the Initiating and Networking funding of the Helmholtz Association (Project Zeitenwende and the Solar Technology Acceleration Platform (Solar TAP)), the program-oriented funding IV of the Helmholtz Association (Materials and Technologies for the Energy Transition, Topic 1: Photovoltaics and Wind Energy, Code: 38.01.04), the German Federal Ministry for Economic Affairs and Climate Action (BMWK) through the projects 27Plus6 (03EE1056B) and SHAPE (03EE1123A), and the Karlsruhe School of Optics and Photonics (KSOP) is gratefully acknowledged. The authors thank the whole “perovskite task force” at KIT for fruitful discussions and assistance.

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