Front-contact passivation through 2D/3D perovskite heterojunctions enables efficient bifacial perovskite/silicon tandem solar cells

Surface passivation by thin-slab 2D perovskites is an effective method to suppress interfacial carrier recombination of 3D metal halide perovskite photoabsorbers. However, improving device performance by integrating such 2D/3D perovskite heterojunctions in the sunward, transparent contacts of perovskite solar cells is not evident due to the high exciton binding energies of phase-pure 2D perovskites, which may result in inefficient free-carrier generation and collection. Here, we overcome this challenge by tuning the dimensionality of 2D perovskites via structural isomers of butylammonium (BA) as a small organic cation, occupying the A-site of the 2D perovskite lattice. The discontinuous iso-BA-based 2D crystals on the 3D perovskite surface yield improved interfacial passivation and enhanced hole extraction. Besides an increased open circuit voltage, this remarkably leads to an enhanced photocurrent (similar to 1 mA cm (-2)) compared with control perovskite solar cells, resulting in bifacial perovskite/silicon tandem solar cells with power generation densities >27 mW cm (-2).