From 2D to 3D: A green solvent system for templated sequential deposition of efficient and stable formamidinium lead triiodide

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From 2D to 3D: A green solvent system for templated sequential deposition of efficient and stable formamidinium lead triiodideBenjamin Gallant a, b, Philippe Holzhey a, Joel Smith a, Saqlain Choudhary a, Karim Elmestekawy a, Henry Snaith aa Department of Physics, University of Oxford, Clarendon Laboratory, Parks Road, OX1 3PU, United Kingdomb School of Chemistry, University of Birmingham, Birmingham, UKInternational Conference on Hybrid and Organic PhotovoltaicsProceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV24)València, Spain, 2024 May 12th - 15thOrganizer: Bruno EhrlerOral, Benjamin Gallant, presentation 032DOI: https://doi.org/10.29363/nanoge.hopv.2024.032Publication date: 6th February 2024Perovskite solar cells (PSCs) offer an efficient, inexpensive alternative to current photovoltaic technologies. However, solution-processing PSCs involves volatilising large volumes of toxic solvents, presenting significant challenges for industrial-scale production. Moreover, perovskite materials are compositionally unstable under operational conditions. Here we employ a novel low-toxicity, biorenewable solvent system to process a range of 2D Ruddlesden Popper perovskite (RPP) compositions. We demonstrate that such 2D RPPs act as highly effective solid-state 'templates' for subsequent solution-processed conversion to α-formamidinium lead triiodide (α-FAPbI3). By tracking the evolution of excitonic photoluminescence from the material progressively throughout conversion we observe the sequence of 2D perovskite intermediates via which this transformation proceeds. It is demonstrated that precise control of the 2D RPP template's phase-composition is of paramount importance to obtain the favourable optoelectronic and material properties of 2D-templated α-FAPbI3. From these findings we propose a 'templated' growth regime in which the inorganic haloplumbate scaffold of the 2D perovskite is retained during conversion and is effective in templating the subsequent growth of low-defect, large-grain 3D perovskite materials. Optical-pump terahertz-probe spectroscopy reveals an electron-hole mobility in excess of 60 cm2 V-1 s-1 for the optimised 3D perovskite, which is among the highest recorded for thin-film α-FAPbI3. Concurrently, an order of magnitude improvement in charge carrier lifetime compared to conventionally processed α-FAPbI3 leads to a carrier diffusion length of 5.3 ± 0.2 μm in our material. Moreover, incorporation of 2D-templated α-FAPbI3 layers into PSCs yields power conversion efficiencies of >21 %. 2D-templated α-FAPbI3 demonstrates substantially improved stability in comparison to other state-of-the-art perovskite compositions. We find remarkably improved thermal stability of FAPbI3 made by our route, which we show is due to the combined novel solvent and templated growth mechanisms; retention of low-volatility solvents (e.g. DMF, DMSO) is avoided, while degradation of the FA+ cation into sym-triazine is substantially reduced. As a result, PSCs based on 2D-templated FAPbI3 show no degradation after 2,000 hours at 85 °C and 85% relative humidity (ISOS-D-3). Moreover, the isolated FAPbI3 thin film material demonstrates heat and light stability of over 3,500 hours and, once incorporated in PSCs, these devices show champion t80 stability of >800 hours in 85 °C, 1 sun equivalent light (ISOS-L-2). © FUNDACIO DE LA COMUNITAT VALENCIANA SCITOnanoGe is a prestigious brand of successful science conferences that are developed along the year in different areas of the world since 2009. Our worldwide conferences cover cutting-edge materials topics like perovskite solar cells, photovoltaics, optoelectronics, solar fuel conversion, surface science, catalysis and two-dimensional materials, among many others.MATSUSPreviously nanoGe Spring Meeting (NSM) and nanoGe Fall Meeting (NFM), MATSUS is a multiple symposia conference focused on a broad set of topics of advanced materials preparation, their fundamental properties, and their applications, in fields such as renewable energy, photovoltaics, lighting, semiconductor quantum dots, 2-D materials synthesis, charge carriers dynamics, microscopy and spectroscopy semiconductors fundamentals, etc.International Conference on Hybrid and Organic PhotovoltaicsInternational Conference on Hybrid and Organic Photovoltaics (HOPV) is celebrated yearly in May. The main topics are the development, function and modeling of materials and devices for hybrid and organic solar cells. 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