How Deep Hole Traps Affect the Charge Dynamics and Collection in Bare and Bilayers of Methylammonium Lead Bromide

[Image: see text] Wide-band-gap perovskites such as methylammonium lead bromide (MAPB) are promising materials for tandem solar cells because of their potentially high open-circuit voltage, which is yet still far below the maximum limit. The relatively short charge-carrier lifetimes deduced from time-resolved photoluminescence (TRPL) measurements seem in strong contrast with the long lifetimes observed with time-resolved photoconductance measurements. This is explained by a large amount of hole defect states, N(T) > 10(16) cm(–3), in spin-coated layers of MAPB residing at or near the grain boundaries. The introduction of hypophosphorous acid (HPA) increases the average grain size by a factor of 3 and reduces the total concentration of the trap states by a factor of 10. The introduction of HPA also increases the fraction of initially generated holes that undergo charge transfer to the selective contact, Spiro-OMeTAD (SO), by an order of magnitude. In contrast to methylammonium lead iodide (MAPI)/SO bilayers, a reduction of the carrier lifetime is observed in MAPB/SO bilayers, which is attributed to the fact that injected holes undergo interfacial recombination via these trap states. Our findings provide valuable insight into the optoelectronic properties of bromide-containing lead halide perovskites essential for designing efficient tandem solar cells.