The impact of interfacial quality and nanoscale performance disorder on the stability of alloyed perovskite solar cells

Kyle Frohna, Cullen Chosy, Amran Al-Ashouri, Florian Scheler, Yu-Hsien Chiang, Milos Dubajic, Julia E. Parker, Jessica M. Walker, Lea Zimmermann, Thomas A. Selby, Yang Lu, Bart Roose, Steve Albrecht, Miguel Anaya () and Samuel D. Stranks ()
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Kyle Frohna: University of Cambridge
Cullen Chosy: University of Cambridge
Amran Al-Ashouri: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Florian Scheler: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Yu-Hsien Chiang: University of Cambridge
Milos Dubajic: University of Cambridge
Julia E. Parker: Harwell Science and Innovation Campus
Jessica M. Walker: Harwell Science and Innovation Campus
Lea Zimmermann: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Thomas A. Selby: University of Cambridge
Yang Lu: University of Cambridge
Bart Roose: University of Cambridge
Steve Albrecht: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Miguel Anaya: University of Cambridge
Samuel D. Stranks: University of Cambridge

Nature Energy, 2025, vol. 10, issue 1, 66-76

Abstract: Abstract Microscopy provides a proxy for assessing the operation of perovskite solar cells, yet most works in the literature have focused on bare perovskite thin films, missing charge transport and recombination losses present in full devices. Here we demonstrate a multimodal operando microscopy toolkit to measure and spatially correlate nanoscale charge transport losses, recombination losses and chemical composition. By applying this toolkit to the same scan areas of state-of-the-art, alloyed perovskite cells before and after extended operation, we show that devices with the highest macroscopic performance have the lowest initial performance spatial heterogeneity—a crucial link that is missed in conventional microscopy. We show that engineering stable interfaces is critical to achieving robust devices. Once the interfaces are stabilized, we show that compositional engineering to homogenize charge extraction and to minimize variations in local power conversion efficiency is critical to improve performance and stability. We find that in our device space, perovskites can tolerate spatial disorder in chemistry, but not charge extraction.

Date: 2025
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DOI: 10.1038/s41560-024-01660-1

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