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We report a thienyl\u2010based self\u2010assembled monolayer (SAM) as an additive in perovskite inks that templates preferential (111) perovskite crystallization. Besides, this SAM is found to spontaneously segregate at perovskite grain boundaries, where strong Pb\u2010S bonding establishes a stable passivating interlayer while the conjugated thienyl moiety facilitates the regulation of energy band alignment. Implemented in perovskite\/TOPCon tandem solar cells, this approach yields a champion power conversion efficiency of 33.00% (certified 32.56%). Crucially, the tandem devices demonstrate substantially improved operational stability, especially for photothermal stress, retaining &gt; 89.8% of initial performance after 1000 h of continuous operation at 65\u00b0C under 1\u2010sun illumination, validating the critical role of thienyl\u2010based SAM in stabilizing perovskite\u2010based tandem photovoltaics.<\/jats:p>","DOI":"10.1002\/anie.5241611","type":"journal-article","created":{"date-parts":[[2026,8,25]],"date-time":"2026-08-25T15:16:47Z","timestamp":1787671007000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Thienyl Self\u2010Assembled Molecule Enabled Stable Perovskite\/TOPCon Silicon Tandem"],"prefix":"10.1002","volume":"65","author":[{"given":"Daoyong","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Silicon and Advanced Semiconductor Materials and School of Materials Science &amp; Engineering Zhejiang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhifen","family":"Huang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Silicon and Advanced Semiconductor Materials and School of Materials Science &amp; Engineering Zhejiang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3181-6873","authenticated-orcid":false,"given":"Zuozuo","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Silicon and Advanced Semiconductor Materials and School of Materials Science &amp; Engineering Zhejiang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ruilin","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Silicon and Advanced Semiconductor Materials and School of Materials Science &amp; Engineering Zhejiang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenbo","family":"Lv","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Silicon and Advanced Semiconductor Materials and School of Materials Science &amp; Engineering Zhejiang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xingqi","family":"Fu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Silicon and Advanced Semiconductor Materials and School of Materials Science &amp; Engineering Zhejiang University  Hangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jungan","family":"Wang","sequence":"additional","affiliation":[{"name":"Research and Development (R&amp;D) Department Zhejiang Jinko Solar Co. 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