Crystallization of Pure-phase Halide Perovskite Films and Strategies for Optimization
Weiwei Zuo a
a Institute for Photovoltaics (ipv), University of Stuttgart, Germany
Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV25)
Roma, Italy, 2025 May 12th - 14th
Organizers: Filippo De Angelis, Francesca Brunetti and Claudia Barolo
Poster, Weiwei Zuo, 015
Publication date: 17th February 2025

After more than ten years of rapid development, the efficiency of perovskite solar cells (PSCs) has already exceeded 26% in the laboratory. Many companies have begun to set up production lines for PSCs in the hope of mass-producing modules, and mature products are just around the corner. However, due to the gap between the harsh device fabrication conditions in the laboratory and the industrial production environment, module samples are still limited by the long-term stability of the device. Therefore, in addition to improving the device fabrication process, a thorough understanding of the crystallization mechanism of perovskite materials is an important part of improving device stability from a manufacturing perspective. 
Generally speaking, the controllable crystallization rate of perovskite enables the production of high-quality films, resulting in high performance solar cells. Our work shows that FAPbI3 has the longest crystallization formation time of all the pure phases of perovskite and can therefore be used to obtain films with low defect density. However, it tends to form the hexagonal non-perovskite polymorph, making it challenging for photovoltaic applications. After a thorough discussion of the perovskite crystallization process, MACl is selected as the crystallizing agent to modulate the intermediate phase and obtain a controllable crystallization rate to produce black phase perovskite films. In addition, MABr is used to heal defects and passivate FAPbI3 to obtain air-stable films. The perovskite solar cell produced using this strategy has an efficiency of 23.0%. [1]
Based on the concern that MABr may affect the growth of pure phase perovskites, we introduce (the green) dimethyl sulfide (DMS) as a novel nucleation trigger for perovskite films, uniquely combining high coordination and low vapor pressure. More specifically, DMS is more coordinative than all currently used solvents and thus effectively replaces them, including DMSO, during film formation. Crucially, DMS also has one of the highest vapor pressures reported in the literature, so it effectively leaves the thin film shortly after formation. This gives DMS universal applicability: DMS replaces other solvents by coordinating more strongly, and removes itself once film formation is complete. To demonstrate this novel coordination chemistry approach, we process MAPbI3 PSCs, typically dissolved in hard-to-remove (and green) DMSO, achieving 21.6% efficiency, one of the highest reported efficiencies for this system. This work provides a universal strategy to control perovskite crystallization using coordination chemistry and heralds the revival of perovskite compositions with pure DMSO, such as MAPbI3. [2]

 

M. S. thanks the German Research Foundation (DFG) for funding (SPP2196, 431314977/GRK 2642). M. S. acknowledges funding by ProperPhotoMile. Project ProperPhotoMile is supported under the umbrella of SOLAR-ERA.NET Cofund 2 by The Spanish Ministry of Science and Education and the AEI under the project PCI2020-112185 and CDTI project number IDI-20210171; the Federal Ministry for Economic Affairs and Energy on the basis of a decision by the German Bundestag project number FKZ 03EE1070B and FKZ 03EE1070A and the Israel Ministry of Energy with project number 220-11-031. SOLAR-ERA.NET is supported by the European Commission within the EU Framework Programme for Research and Innovation HORIZON 2020 (Cofund ERA-NET Action, No. 786483). M. S. acknowledges funding from the European Research Council under the Horizon Europe programme (LOCAL-HEAT, grant agreement no. 101041809). M. S. acknowledges funding from the German Bundesministerium für Bildung and Forschung (BMBF), project “NETPEC” (01LS2103E).

© FUNDACIO DE LA COMUNITAT VALENCIANA SCITO
We use our own and third party cookies for analysing and measuring usage of our website to improve our services. If you continue browsing, we consider accepting its use. You can check our Cookies Policy in which you will also find how to configure your web browser for the use of cookies. More info