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In particular, the molecular orientation and packing of self\u2010assembled monolayers (SAMs) can significantly influence perovskite film formation and device performance. Here, we rationally design a series of carbazole\u2010based SAMs and identify a bicarbazole\u2010core molecule, 9,9\u2010DCz, that adopts a predominantly upright orientation on indium tin oxide (ITO), in contrast to the conventional flat\u2010lying alignment. This vertical configuration facilitates denser surface coverage, favorable energy\u2010level alignment, and reduced non\u2010radiative recombination in the WBG perovskite layer. As a result, we achieve a certified power conversion efficiency (PCE) of 19.95% (champion 20.81%) for the WBG subcell (1.77\u00a0eV, 0.0396 cm\n                    <jats:sup>2<\/jats:sup>\n                    ), and 28.59% for the all\u2010PSK tandem device. Our findings indicate that upright SAMs orientation as an effective design principle for high\u2010performance WBG and tandem perovskite photovoltaics.\n                  <\/jats:p>","DOI":"10.1002\/adma.202521898","type":"journal-article","created":{"date-parts":[[2026,3,28]],"date-time":"2026-03-28T08:19:51Z","timestamp":1774685991000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["\u201cStanding up\u201d SAMs for Efficient Wide Bandgap and All\u2010Perovskite Tandem Solar Cells"],"prefix":"10.1002","volume":"38","author":[{"given":"Chongyu","family":"Zhong","sequence":"first","affiliation":[{"name":"State Key Laboratory of Flexible Electronics (KLOFE) Institute of Advanced Materials (IAM) &amp; School of Flexible Electronics (Future Technologies) Nanjing Tech University (Nanjing Tech)  Nanjing Jiangsu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junbo","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Flexible Electronics (KLOFE) Institute of Advanced Materials (IAM) &amp; School of Flexible Electronics (Future Technologies) Nanjing Tech University (Nanjing Tech)  Nanjing Jiangsu China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhangsheng","family":"Shi","sequence":"additional","affiliation":[{"name":"Department of Chemistry City University of Hong Kong  Hong Kong SAR P. 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