How crystallization additives govern halide perovskite grain growth

Timo Maschwitz, Lena Merten, Feray Ünlü, Martin Majewski, Fatemeh Haddadi Barzoki, Zijin Wu, Seren Dilara Öz, Cedric Kreusel, Manuel Theisen, Pang Wang, Maximilian Schiffer, Gianluca Boccarella, Gregor Marioth, Henrik Weidner, Sarah Schultheis, Tim Schieferstein, Dawid Gidaszewski, Zavkiddin Julliev, Ekaterina Kneschaurek, Valentin Munteanu, Ivan Zaluzhnyy, Florian Bertram, Anaël Jaffrès, Junjie He, Nigmat Ashurov, Martin Stolterfoht, Christian M. Wolff, Eva Unger, Selina Olthof, Geert Brocks, Shuxia Tao, Helen Grüninger, Olivier J. J. Ronsin, Jens Harting, Andreas F. Kotthaus (), Stefan F. Kirsch, Sanjay Mathur, Alexander Hinderhofer (), Frank Schreiber, Thomas Riedl () and Kai Oliver Brinkmann ()
Additional contact information
Timo Maschwitz: University of Wuppertal
Lena Merten: University of Tübingen
Feray Ünlü: University of Cologne
Martin Majewski: Forschungszentrum Jülich
Fatemeh Haddadi Barzoki: University of Bayreuth
Zijin Wu: Department of Applied Physics and Science Education, Eindhoven University of Technology
Seren Dilara Öz: University of Wuppertal
Cedric Kreusel: University of Wuppertal
Manuel Theisen: University of Wuppertal
Pang Wang: University of Wuppertal
Maximilian Schiffer: University of Wuppertal
Gianluca Boccarella: University of Wuppertal
Gregor Marioth: University of Wuppertal
Henrik Weidner: University of Wuppertal
Sarah Schultheis: University of Wuppertal
Tim Schieferstein: University of Wuppertal
Dawid Gidaszewski: Eindhoven Institute for Renewable Energy Systems (EIRES) Eindhoven University of Technology
Zavkiddin Julliev: Academy of Science of the Republic of Uzbekistan
Ekaterina Kneschaurek: University of Tübingen
Valentin Munteanu: University of Tübingen
Ivan Zaluzhnyy: University of Tübingen
Florian Bertram: Deutsches Elektronen-Synchrotron DESY
Anaël Jaffrès: Ecole Polytechnique Fédérale de Lausanne (EPFL), Photovoltaics and Thin-Film Electronics Laboratory
Junjie He: University of Wuppertal
Nigmat Ashurov: Academy of Science of the Republic of Uzbekistan
Martin Stolterfoht: The Chinese University of Hong Kong
Christian M. Wolff: Ecole Polytechnique Fédérale de Lausanne (EPFL), Photovoltaics and Thin-Film Electronics Laboratory
Eva Unger: Helmholtz-Zentrum Berlin für Materialen und Energie GmbH
Selina Olthof: University of Wuppertal
Geert Brocks: Department of Applied Physics and Science Education, Eindhoven University of Technology
Shuxia Tao: Department of Applied Physics and Science Education, Eindhoven University of Technology
Helen Grüninger: University of Bayreuth
Olivier J. J. Ronsin: Forschungszentrum Jülich
Jens Harting: Forschungszentrum Jülich
Andreas F. Kotthaus: Bergische Universität Wuppertal
Stefan F. Kirsch: Bergische Universität Wuppertal
Sanjay Mathur: University of Cologne
Alexander Hinderhofer: University of Tübingen
Frank Schreiber: University of Tübingen
Thomas Riedl: University of Wuppertal
Kai Oliver Brinkmann: University of Wuppertal

Nature Communications, 2025, vol. 16, issue 1, 1-16

Abstract: Abstract The preparation of perovskite solar cells from the liquid phase is a cornerstone of their immense potential. However, a clear relationship between the precursor ink and the formation of the resulting perovskite is missing. Established theories, such as heterogeneous nucleation and lead complex colloid formation, often prove unreliable, which has led to an overreliance on heuristics. Most high-performing perovskites use additives to control crystallization. Their role during crystallization is, however, elusive. Here, we provide evidence that typical crystallization additives do not predominantly impact the nucleation phase but rather facilitate coarsening grain growth by increasing ion mobility across grain boundaries. Drawing from the insights of our broad, interdisciplinary study that combines ex and in situ characterization methods, devices, simulations, and density function theory calculation, we propose a concept that proves valid for various additives and perovskite formulations. Moreover, we establish a direct link between additive engineering and perovskite post-processing, offering a unified framework for advancing material design and process engineering.

Date: 2025
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DOI: 10.1038/s41467-025-65484-7

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