All-perovskite–based polycrystalline thin-film tandem solar cells have the potential to deliver efficiencies of >30%. However, the performance of all-perovskite–based tandem devices has been limited by the lack of high-efficiency, low–band gap tin-lead (Sn-Pb) mixed-perovskite solar cells (PSCs). We found that the addition of guanidinium thiocyanate (GuaSCN) resulted in marked improvements in the structural and optoelectronic properties of Sn-Pb mixed, low–band gap (~1.25 electron volt) perovskite films. The films have defect densities that are lower by a factor of 10, leading to carrier lifetimes of greater than 1 microsecond and diffusion lengths of 2.5 micrometers. These improved properties enable our demonstration of >20% efficient low–band gap PSCs. When combined with wider–band gap PSCs, we achieve 25% efficient four-terminal and 23.1% efficient two-terminal all-perovskite–based polycrystalline thin-film tandem solar cells.

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Recent achievements of 2D perovskites for various optoelectronic applications along with their basic properties and future opportunities are discussed.

Maximizing the power conversion efficiency (PCE) of perovskite/silicon tandem solar cells that can exceed the Shockley-Queisser single-cell limit requires a high-performing, stable perovskite top cell with a wide bandgap. We developed a stable perovskite solar cell with a bandgap of ~1.7 electron volts that retained more than 80% of its initial PCE of 20.7% after 1000 hours of continuous illumination. Anion engineering of phenethylammonium-based two-dimensional (2D) additives was critical for controlling the structural and electrical properties of the 2D passivation layers based on a lead iodide framework. The high PCE of 26.7% of a monolithic two-terminal wide-bandgap perovskite/silicon tandem solar cell was made possible by the ideal combination of spectral responses of the top and bottom cells.

This work shows a bimolecular additive engineering approach to prepare highly efficient wide-band-gap perovskite solar cells. The coupling of PEA + and SCN À provides a synergistic effect that overcomes growth challenges with either additive individually and improves perovskite quality with enhanced crystallinity, reduced defect density, and improved carrier mobility and lifetime. When coupling a semitransparent wide-band-gap perovskite top cell with a low-band-gap CIGS bottom cell, we achieve a 25.9%-efficient polycrystalline perovskite/CIGS 4-terminal thinfilm tandem solar cell.

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The first bottom-up solution-processed perovskite–perovskite tandem solar cell has been successfully fabricated via an optimized charge recombination layer comprising spiro-OMeTAD/PEDOT:PSS/PEI/PCBM:PEI. The as-fabricated tandem device delivers an open voltage of up to 1.89 V, close to the sum of the two perovskite subcells.