Understanding the morphology formation of photoactive layers in perovskite and organic solar cells with the help of advanced simulations
Olivier Ronsin a b, Jens Harting a b c
a Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (HI ERN), Forschungszentrum Jülich GmbH (FZJ), Immerwahrstraße, 2, Erlangen, Germany
b Department of Chemical and Biological Engineering, Friedrich-Alexander-Universität Erlangen- Nürnberg
c Department of Physics, Friedrich-Alexander-Universität Erlangen- Nü rnberg
International Conference on Hybrid and Organic Photovoltaics
Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV23)
London, United Kingdom, 2023 June 12th - 14th
Organizers: Tracey Clarke, James Durrant and Trystan Watson
Oral, Olivier Ronsin, presentation 043
DOI: https://doi.org/10.29363/nanoge.hopv.2023.043
Publication date: 30th March 2023

The processing conditions strongly impact the morphology of the photoactive layers in perovskite (PSC) and organic solar cells (OSC), and thus their performances. However, the process-structure relationship remains insufficiently understood. In this talk, we will show how the absorber layer morphology formation of solution-processed solar cells can be simulated, using a recently developed theoretical model. For the first time, this allows to investigate the interplay between all the relevant physical processes (evaporation, crystal nucleation and growth, liquid demixing, composition-dependent kinetic properties), within a single coherent framework.
The approach will be illustrated for OSC based on simulations of the morphology formation for a well-documented polymer-small molecule bulk-heterojunction. The comparison with previously reported in-situ characterization of the drying structure is very convincing: the morphology formation pathways, crystallization kinetics, and final morphology are in line with experimental results. The final morphology is a subtle mixture of pure crystalline donor and acceptor phases, pure and mixed amorphous domains, which depends on the process parameters and material properties. For PSC, simulations showing the impact of the evaporation rate on the final crystalline structure will be shown. The results regarding substrate coverage, film roughness, crystals sizes are in excellent agreement with experimental results, and the conditions for obtaining high-quality films will be discussed.
The major innovative value of the work is that the process-structure relationship in solution-processed photovoltaics can now be investigated with comprehensive computer simulations instead of costly trial and error experiments. This is a worldwide unique approach that represents an outstanding opportunity for the PV-community in order to identify new design rules for ink formulation and processing conditions.

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