To bring hybrid lead halide perovskite solar cells toward the Shockley-Queisser limit requires lowering the band gap while simultaneously increasing the open-circuit voltage. This, to some extent divergent objective, may demand the use of largecations to obtain a perovskite with larger lattice parameter together with a large crystalsize to minimize interface nonradiative recombination. When applying the two-stepmethod for a better crystal control, it is rather challenging to fabricate perovskites withFA+cations, given the small penetration depth of such large ions into a compact PbI2film. In here, to successfully incorporate such large cations, we used a high-concentration solution of the organic precursor containing small Cl-anions achieving,via a solvent annealing-controlled dissolution-recrystallization, larger than 1µmperovskite crystals in a solar cell. This solar cell, with a largely increasedfluorescencequantum yield, exhibited an open-circuit voltage equivalent to 93% of thecorresponding radiative limit one. This, together with the low band gap achieved(1.53 eV), makes the fabricated perovskite cell one of the closest to the Shockley-Queisser optimum.

Peer Reviewed