Coordination Chemistry Limits Crystallization of Lead Halide Perovskites
Antonio Guerrero a
NIPHO
Proceedings of Perovskite Thin Film Photovoltaics (ABXPV16)
Barcelona, Spain, 2016 March 3rd - 4th
Organizers: Emilio Palomares and Nam-Gyu Park
Oral, Antonio Guerrero, presentation 006
Publication date: 14th December 2015

Photovoltaic perovskites field is slowly shifting from highly disordered1 perovskite solar cells towards generation of single crystal2 devices which can ultimately provide lower energy losses. In this work we investigate crystallization of lead halide perovskite from first principles by a combination of theoretical and experimental approach. Competition between iodides with solvent molecules to coordinate lead atoms will determine the species present during perovskite nucleation and growth. Low complexity DFT calculations help to understand solvent coordination ability and can be used as a tool to screen suitable solvents. Highly coordinating solvents such as DMSO will form partially covalent bonds with lead retarding crystallization kinetics and its subsequent removal may be difficult. Poorly coordinating solvents like GBL will not be able to stabilize PbI3- moieties enabling a fast reaction with the methyl ammonium cation. The theoretical approach is confirmed by the synthesis of pure material and generation in films. Importantly, water present in environmental humidity can be regarded as an additive which retards perovskite crystallization. Moisture will have a healing effect which avoids pinholes for intermediate coordinating solvents like DMF. The information presented here is crucial to understand crystallization of perovskite to further increase device efficiencies and improve lab-to-lab reproducibility.

References

1-Guerrero et al APL, 2014, 133902

2-Saidaminov et al. Nat. Commun. 2015, 6.



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