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A primary bottleneck is the formation of unfavorable buried interfaces and energy level misalignment, often caused by inadequate self\u2010assembled monolayers (SAMs) on indium tin oxide\/nickel oxide (ITO\/NiO\n                    <jats:sub>x<\/jats:sub>\n                    ) substrates used for the front perovskite subcell. To address this critical issue, two dimeric SAM materials, named DTh\u20104PACz and DPh\u20104PACz, were synthesized using thiophene and benzene linkers, respectively, to connect two carbazole\u2010derived molecules. The DPh\u20104PACz\u2010modified ITO\/NiO\n                    <jats:sub>x<\/jats:sub>\n                    substrate exhibits an improved buried interface, leading to wide\u2010bandgap (WBG) perovskites with enhanced crystallinity and reduced defect density compared to the DTh\u20104PACz\u2010based counterpart. Besides, DPh\u20104PACz possesses enhanced conductivity and forms better energy level alignment with the WBG perovskites. Consequently, the best\u2010performing WBG perovskite solar cell (PSC) based on DPh\u20104PACz achieves a higher PCE of 18.78%, compared to 16.77% for the DTh\u20104PACz\u2010based PSC. By integrating the DPh\u20104PACz\u2010based 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\u20104PACz\u2010based POTSC shows enhanced thermal and light stability. This work provides an effective dimeric SAM material design strategy for efficient and stable PSCs and POTSCs.\n                  <\/jats:p>","DOI":"10.1002\/anie.5905435","type":"journal-article","created":{"date-parts":[[2026,4,17]],"date-time":"2026-04-17T06:29:28Z","timestamp":1776407368000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Dimeric Self\u2010Assembled Monolayer Materials for High\u2010Performance Perovskite and Perovskite\/Organic Tandem Solar Cells"],"prefix":"10.1002","volume":"65","author":[{"given":"Wenwu","family":"Zhou","sequence":"first","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry College of Engineering and Applied Sciences Nanjing University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huixiang","family":"Jiao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Coordination Chemistry College of Engineering 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