Dually Modified Wide-Bandgap Perovskites by Phenylethylammonium Acetate toward Highly Efficient Solar Cells with Low Photovoltage Loss

Wide-bandgap perovskites as a class of promising top-cell materials have shown great promise in constructing efficient perovskite-based tandem solar cells, but their intrinsic relatively low radiative efficiency results in a large open-circuit voltage (V_OC) deficit and thereby limits the whole device performance. Reducing film flaws or optimizing interfacial energy level alignments in wide-bandgap perovskite devices can efficiently inhibit nonradiative recombination to boost device V_OC and efficiency. However, the simultaneous regulation on both sides and their underlying mechanism are less explored. Herein, a bifunctional modification approach is proposed to optimize the wide-bandgap perovskite surface with an ultrathin layer of phenylethylammonium acetate (PEAAc) to synchronously decrease the surface imperfection and mitigate the interfacial energy barrier. This treatment effectively heals under-coordinated surface defects through the formation of chemical interaction between the perovskite and PEAAc, bringing about a much slower charge trapping process and dramatically decreasing nonradiative recombination losses. Meanwhile, the passivation-induced upshifted Fermi level of the perovskite contributes to accelerated electron extraction and larger Fermi-level splitting under illumination. Consequently, the PEAAc-modified wide-bandgap (1.68 eV) device achieves an optimal efficiency of 20.66% with a high V_OC of 1.25 V, among the highest reported V_OC values for wide-bandgap perovskite devices, enormously outperforming that (18.86% and 1.18 V) of the device without passivation. In addition, the radiative limit of V_OC for both cells is determined to be 1.42 V, delivering nonradiative recombination losses of 0.24 and 0.17 V for the control and PEAAc-modified devices, respectively. These results highlight the significance of the bifunctional modification strategy in achieving high-performance wide-bandgap perovskite devices.