Interface carrier recombination currently hinders the performance of hybrid organic-silicon heterojunction solar cells for high-efficiency low-cost photovoltaics. Here, we introduce an intermediate 1,1-bis[(di-4-tolylamino)phenyl]cyclohexane (TAPC) layer into hybrid heterojunction solar cells based on silicon nanowires (SiNWs) and conjugate polymer poly(3,4-ethylenedioxy-thiophene):poly(styrenesulfonate) (PEDOT:PSS). The highest power conversion efficiency reaches a record 13.01%, which is largely ascribed to the modified organic surface morphology and suppressed saturation current that boost the open-circuit voltage and fill factor. We show that the insertion of TAPC increases the minority carrier lifetime because of an energy offset at the heterojunction interface. Furthermore, X-ray photoemission spectroscopy reveals that TAPC can effectively block the strong oxidation reaction occurring between PEDOT:PSS and silicon, which improves the device characteristics and assurances for reliability. These learnings point toward future directions for versatile interface engineering techniques for the attainment of highly efficient hybrid photovoltaics.

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In this study, an efficient and stable large‐area blade‐coated organic solar cell (OSC) module with an active area of 216 cm2 (16 elementary cells connected in series) is demonstrated by combining appropriate thermal annealing treatment with the use of 4,4′‐(((methyl(4‐sulphonatobutyl)ammonio)bis(propane‐3,1‐diyl))bis(dimethyl‐ammoniumdiyl))bis‐(butane‐1‐sulfonate) (MSAPBS) as the cathode interfacial layer. For the opaque device using poly[4,8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)benzo[1,2‐b;4,5‐b′]dithiophene‐2,6‐diyl‐alt‐(4‐(2‐ethylhexyl)‐3‐fluorothieno[3,4‐b]thiophene‐)‐2‐carboxylate‐2‐6‐diyl)] (PBDTTT‐EFT (PTB7‐Th)):[6,6]‐phenyl C71‐butyric acid methyl ester (PC71BM) blend film as the active layer, the power conversion efficiency (PCE) of 5.6% is achieved under AM 1.5G solar light illumination. Very encouragingly, our strategy can be applicable for semitransparent OSCs, and a remarkable PCE up to 4.5% is observed. To the best of our knowledge, the PCE of 5.6% for opaque device and 4.5% for semitransparent device represent the highest PCE ever reported for OSCs with the active area exceeding 100 cm2. The devices also show an impressive stability under outdoor environment, where the efficiency decay is less than 30% for 60 days. Our findings can pave the way toward the development of organic solar cell modules with high performance and long‐term stability.

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