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High efficiency combined with transformative roll-to-roll (R2R) printability makes metal halide perovskite-based solar cells the most promising solar technology to address the terawatt challenge of the future energy demand. However, translation from lab-scale deposition solution processing techniques to large-scale R2R methods has typically led to reduced photovoltaic performance. Here, we demonstrate large-scale, highly crystalline, uniaxially oriented, smooth perovskite films printed at room temperature and in the ambient environment. Confirmed with high speed in situ X-ray diffraction measurements, the perovskite films reach 98% of relative crystallinity at room temperature and display high texture within 1 s of the coating. We demonstrate an all-blade-coated metal halide perovskite cell with power conversion efficiency (PCE) up to 19.6%, a slot-die coated cell with a PCE of 17.3%, and a partially R2R slot-die coated flexible glass-based cell efficiency of 14.1%. The developed printing method can be applied to diverse perovskite compositions, enabling a variety of bandgaps to pave the way for the future R2R printing of highly efficient perovskite–perovskite tandem cells.

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For halide perovskite solar cells (PSCs) to fulfill their vast potential for combining low-cost, high efficiency, and high throughput production they must be scaled using a truly transformative method, such as roll-to-roll processing. Bringing this reality closer to fruition, the present work demonstrates flexible perovskite solar cells with 18.1% power conversion efficiency on flexible Willow Glass substrates. We highlight the importance of the transparent conductive oxide (TCO) layers on device performance by studying various TCOs. While tin-doped indium oxide (ITO) and indium zinc oxide (IZO) based PSC devices demonstrate high photovoltaic performances, aluminum-doped zinc oxide (AZO) based devices underperformed in all device parameters. Analysis of X-ray photoemission spectroscopy data shows that the stoichiometry of the perovskite film surface changes dramatically when it is fabricated on AZO, demonstrating the importance of the substrate in perovskite film formation.

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