Dimeric Self‐Assembled Monolayer Materials for High‐Performance Perovskite and Perovskite/Organic Tandem Solar Cells

substrate exhibits an improved buried interface, leading to wide-bandgap (WBG) perovskites with enhanced crystallinity and reduced defect density compared to the DTh-4PACz-based counterpart. Besides, DPh-4PACz possesses enhanced conductivity and forms better energy level alignment with the WBG perovskites. Consequently, the best-performing WBG perovskite solar cell (PSC) based on DPh-4PACz achieves a higher PCE of 18.78%, compared to 16.77% for the DTh-4PACz-based PSC. By integrating the DPh-4PACz-based WBG PSC as the front subcell into POTSCs, the resulting device delivers an exceptional PCE of 26.63% (certified at 26.09%). Moreover, the DPh-4PACz-based POTSC shows enhanced thermal and light stability. This work provides an effective dimeric SAM material design strategy for efficient and stable PSCs and POTSCs.