All-perovskite tandem solar cells are promising for achieving photovoltaics with power conversion efficiencies above the detailed balance limit of single-junction cells, while retaining the low cost, light weight and other advantages associated with metal halide perovskite photovoltaics. However, the efficiency and stability of all-perovskite tandem cells are limited by the Sn–Pb-based narrow-bandgap perovskite cells. Here we show that the formation of quasi-two-dimensional (quasi-2D) structure (PEA)2GAPb2I7 from additives based on mixed bulky organic cations phenethylammonium (PEA+) and guanidinium (GA+) provides critical defect control to substantially improve the structural and optoelectronic properties of the narrow-bandgap (1.25 eV) Sn–Pb perovskite thin films. This 2D additive engineering results in Sn–Pb-based absorbers with low dark carrier density (~1.3 × 1014 cm−3), long bulk carrier lifetime (~9.2 μs) and low surface recombination velocity (~1.4 cm s−1), leading to 22.1%-efficient single-junction Sn–Pb perovskite cells and 25.5%-efficient all-perovskite two-terminal tandems with high photovoltage and long operational stability.
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The work at the National Renewable Energy Laboratory was supported by the US Department of Energy under contract no. DE-AC36-08GO28308 with Alliance for Sustainable Energy, Limited Liability Company, the manager and operator of the National Renewable Energy Laboratory. We acknowledge the support for perovskite synthesis, device fabrication and characterization from the De-risking Halide Perovskite Solar Cells programme of the National Center for Photovoltaics (J.T., Q.J., A.F.P., F.Z., S.P.D., A.E.L., R.M.F., M.Y., J.F.G., J.J.B. and K.Z.) and the support for TRPL characterization and analysis from award no. 34361 (A.J.F. and D.K.) funded by the US Department of Energy, Office of Energy Efficiency and Renewable Energy, Solar Energy Technologies Office. We also acknowledge the support for time-resolved microwave conductivity and Hall effect measurement and analysis from the Center for Hybrid Organic Inorganic Semiconductors for Energy, an Energy Frontier Research Center funded by the Office of Basic Energy Sciences, Office of Science within the US Department of Energy (J.H., H.L. and M.C.B.). Contributions from S.A.J. and M.D.M. were supported by the US Department of Energy’s Office of Energy Efficiency and Renewable Energy under Solar Energy Technologies Office agreement no. DE-EE0008551. The views expressed in the article do not necessarily represent the views of the US Department of Energy or the US government.
M.D.M. is an advisor to Swift Solar. J.T., Q.J. and K.Z. are inventors on a pending provisional patent (US patent application number 63/227,415; by Alliance for Sustainable Energy) related to the 2D cation engineering of Sn-Pb perovskites for tandem solar cell application as discussed in this manuscript.
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Tong, J., Jiang, Q., Ferguson, A.J. et al. Carrier control in Sn–Pb perovskites via 2D cation engineering for all-perovskite tandem solar cells with improved efficiency and stability. Nat Energy 7, 642–651 (2022). https://doi.org/10.1038/s41560-022-01046-1
Nature Energy (2022)