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However, the halide homogenization process readily induces deep\u2010level defects because iodide incorporation into bromide\u2010rich phases is hard to control. Here, we report a bifunctional ammonium salt strategy that achieves sequential defect control during this process. We find that iodide interstitial and antisite incorporation into the perovskite lattice leads to the formation of halide trimer motifs, which constitute a common structural origin of deep\u2010level defects. Our strategy uses 4\u2010(2\u2010aminoethyl)benzenesulfonic acid hydrochloride, where the sulfonic acid group kinetically regulates iodide incorporation within the narrow homogenization window, while the ammonium moiety reconstructs the local atomic configurations of halide trimer motifs, enabling the spontaneous sequential suppression and deactivation of these deep\u2010level defects. This strategy delivers a champion efficiency of 23.81% for MA\u2010free perovskite solar cells and 32.3% for perovskite\/silicon tandem devices, which retain over 90% of their initial efficiency after 1000\u00a0h of continuous illumination in ambient air. This work advances the understanding and molecular control of deep\u2010level defects arising from halide homogenization in wide\u2010bandgap perovskites.<\/jats:p>","DOI":"10.1002\/anie.2375835","type":"journal-article","created":{"date-parts":[[2026,10,2]],"date-time":"2026-10-02T07:33:38Z","timestamp":1790926418000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Bifunctional Molecular Regulation Couples Halide Homogenization With Deep\u2010Level Defect Control in MA\u2010Free Wide\u2010Bandgap Perovskites for Tandem Solar Cells"],"prefix":"10.1002","author":[{"given":"Cong","family":"Sun","sequence":"first","affiliation":[{"name":"Institute of Photoelectronic Thin Film Devices and Technology Renewable Energy Conversion and Storage Center State Key Laboratory of Photovoltaic Materials and Cells Nankai University  Tianjin P. R. 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