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Herein, we employ 3,4,5\u2010trifluorobenzeneboronic acid (3FBBA) as a multifunctional modulator that synergistically interacts with both organic cations and lead\u2010halide octahedra via complementary hydrogen\u2010bonding and coordination interactions, by which 3FBBA fundamentally modulates the formation mechanism of\n                    <jats:italic>\u03b1<\/jats:italic>\n                    \u2010phase perovskite. It transforms the spontaneous, uncontrolled direct crystallization pathway into a well\u2010regulated phase\u2010transition process mediated by highly ordered intermediate phases. These well\u2010structured intermediates act as well\u2010defined pre\u2010structural frameworks to guide the formation of high\u2010quality\n                    <jats:italic>\u03b1<\/jats:italic>\n                    \u2010phase perovskite. Benefiting from this strategy, the resultant WBG perovskite films possess enlarged grain size and reduced defect density, which suppress nonradiative recombination loss and accelerate charge transfer kinetics. As a consequence, a single\u2010junction 1.66 eV WBG perovskite solar cell (PSC) achieves a high\u2010power conversion efficiency (PCE) of 24.09%, while a two\u2010terminal perovskite\/silicon TSC delivers a champion PCE of 33.6%. Notably, the unencapsulated TSC maintains over 90% of its initial PCE throughout 571 h of continuous maximum power point tracking (MPPT) under ambient atmospheric conditions.\n                  <\/jats:p>","DOI":"10.1002\/adma.74784","type":"journal-article","created":{"date-parts":[[2026,8,22]],"date-time":"2026-08-22T09:03:53Z","timestamp":1787389433000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Intermediate\u2010Phase\u2010Mediated Homogeneous Crystallization of Wide\u2010Bandgap Perovskite for Efficient Silicon\/Perovskite Tandem Solar Cells"],"prefix":"10.1002","author":[{"given":"Ruikun","family":"Cao","sequence":"first","affiliation":[{"name":"State Key Laboratory of Fine Chemicals School of Chemistry Frontier Science Center for Smart Materials Dalian University of Technology  Dalian P. R. China"},{"name":"School of Integrated Circuits Dalian University of Technology  Dalian P. R. 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