Role of lead precursors in driving competitive crystallization reactions during the formation of 2D perovskites

Leo Sahaya Daphne Antony^a, Gianluca Grimaldi^a^,^b, Lukas Helmbrecht^a, Arno van der Wejiden^a, Imme Schuringa^a, Juliane Borchert^a^,^b, Bruno Erhler^a, Wim Noorduin^a, Esther Alarcon Llado^a

^aCenter for Nanophotonics, AMOLF, The Netherlands, Science Park, 104, Amsterdam, Netherlands

^bOptoelectronics section, Cavendish Laboratory, University of Cambridge, Cambridge, United Kingdom

Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Spring Meeting 2022 (NSM22)

#ChemNano22. Chemistry of Nanomaterials

Online, Spain, 2022 March 7th - 11th

Organizers: Loredana Protesescu and Maksym Yarema

Contributed talk, Leo Sahaya Daphne Antony, presentation 304
DOI: https://doi.org/10.29363/nanoge.nsm.2022.304
Publication date: 7th February 2022

Hybrid organic–inorganic perovskite semiconductors have triggered a paradigm shift in the field of photovoltaics (PVs). Low dimensional 2D hybrid organic–inorganic lead halide semiconductors have recently attracted major attention [1] owing to the emergence of new photo-physical properties compared to the 3D perovskites, including exciton-phonon coupling, edge state based charge dissociation at grain boundaries and photon confinement [2]. The ionic nature of these layered materials also make them ideal candidates for solution processing into both thin films and nanostructured crystals [3]. Studying the wide range of process parameters in different solution processing techniques like spin coating [4], drop casting [5,6], meniscus coating [7] is important as they greatly influence the crystallization of 2D perovskites. However, this plethora of parameters in solution processing of 2D perovskites are not understood as well as their 3D counterparts.

Here we report the effects of different lead precursors in the crystallization process of 2D perovskite during a simple drop-cast based synthesis. We study the role of lead iodide (PbI₂), lead carbonate (PbCO₃) and lead dioxide (PbO₂) in the crystallization of BA₂PbI₄ perovskite in IPA-based solvent system. Our in-situ observations during the drop-casting process reveal the different crystallization kinetics based on the initial lead precursor. We also observe crystallization of the perovskite either on the substrate or in solution as floating micro-plates or both depending on the type of the precursor. We attribute this behavior to the formation of different co-ordinate complexes based on the initial lead precursor. Upon structural and optical investigation of the synthesized perovskite crystals (on substrate and in solution), we find them to be highly crystalline when compared against the traditionally grown and exfoliated 2D perovskites.

References:

[1] Cao, D. H.; Stoumpos, C. C.; Farha, O. K.; Hupp, J. T.; Kanatzidis, M. G. 2D Homologous Perovskites as Light-Absorbing Materials for Solar Cell Applications. J. Am. Chem. Soc. 2015, 137, 24, 7843–7850.

[2] Gan, Z.; Cheng, Y.; Chen, W.; Loh, K. P.; Jia, B.; Wen, X. Photophysics of 2D Organic-Inorganic Hybrid Lead Halide Perovskites: Progress, Debates, and Challenges. Adv. Sci. 2021, 8, 2001843.

[3] Jagielski, J.; Kumar, S.; Yu, W-Y; Shih, C-J. Layer-controlled two-dimensional perovskites: synthesis and optoelectronics. J. Mater. Chem. C, 2017,5, 5610-5627.

[4] 4. Hoffman, J. M.; Strzalka, J.; Flanders, N. C.; Hadar, I.; Cuthriell, S. A.; Zhang, Q.; Schaller, R. D.; Dichtel, W. R.; Chen, L. X.; Kanatzidis, M. G. In Situ Grazing-Incidence Wide-Angle Scattering Reveals Mechanisms for Phase Distribution and Disorientation in 2D Halide Perovskite Films. Adv. Mater. 2020, 32, 2002812.

[5] Zuo, C., Scully, A. D., Vak, D., Tan, W., Jiao, X., McNeill, C. R., Angmo, D., Ding, L., Gao, M. Self-Assembled 2D Perovskite Layers for Efficient Printable Solar Cells. Adv. Energy Mater. 2019, 9, 1803258.

[6] 6. Grimaldi, G.; Antony, L. S. D.; Helmbrecht, L.; van der Weijden, A.; van Dongen, S. W.; Schuringa, I.; Borchert, J.; Alarcón-Lladó, E.; Noorduin, W. L.; Ehrler. Microstructuring of 2D perovskites via ion-exchange fabrication. B. Appl. Phys. Lett. 2021, 119, 223102.

[7] 7. Wu, Z.; Li, W.; Ye, Y.; Li, X.; Lin, H. Recent progress in meniscus coating for large-area perovskite solar cells and solar modules. Sustainable Energy Fuels, 2021, 5, 1926-1951.

Acknowledgements:

Esther Alarcon Llado and Leo Sahaya Daphne Antony acknowledge the D3N project (Project No. 17972 of the research programme HTSM2019 from the NWO-TTW Domain), which is (partly) financed by the Dutch Research Council (NWO).

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