Efficient Semi-Transparent Wide-Bandgap Perovskite Solar Cells Enabled by Pure-Chloride 2D-Perovskite Passivation

Wide-bandgap (WBG) perovskite solar cells suffer from severe non-radiative recombination and exhibit relatively large open-circuit voltage (V(OC)) deficits, limiting their photovoltaic performance. Here, we address these issues by in-situ forming a well-defined 2D perovskite (PMA)(2)PbCl(4) (phenmethylammonium is referred to as PMA) passivation layer on top of the WBG active layer. The 2D layer with highly pure dimensionality and halide components is realized by intentionally tailoring the side-chain substituent at the aryl ring of the post-treatment reagent. First-principle calculation and single-crystal X-ray diffraction results reveal that weak intermolecular interactions between bulky PMA cations and relatively low cation-halide hydrogen bonding strength are crucial in forming the well-defined 2D phase. The (PMA)(2)PbCl(4) forms improved type-I energy level alignment with the WBG perovskite, reducing the electron recombination at the perovskite/hole-transport-layer interface. Applying this strategy in fabricating semi-transparent WBG perovskite solar cells (indium tin oxide as the back electrode), the V(OC) deficits can be reduced to 0.49 V, comparable with the reported state-of-the-art WBG perovskite solar cells using metal electrodes. Consequently, we obtain hysteresis-free 18.60%-efficient WBG perovskite solar cells with a high V(OC) of 1.23 V. GRAPHICAL ABSTRACT: [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-023-01090-w.