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Herein, two carbazole\u2010based molecules with different halogen atoms (X\u2010OCZ, X = Cl or Br) are developed as efficient interfacial regulators. The halogen effect not only finely modulates the molecular packing, crystallinity, and surface contact potential of the MeO\u20102PACz analogue via self\u2010induced intermolecular interactions but also significantly influences the subsequent crystal growth of perovskite, thus resulting in the formation of high\u2010quality films with enhanced crystallinity, improved energy level alignment, and depressed non\u2010radiative recombination. Importantly, the Cl\u2010OCZ\u2010mediated device exhibits a minimal interfacial carrier transport energy barrier of 0.10\u00a0eV and an impressive charge collection efficiency of 93.6%. Moreover, the target device (aperture area: 0.09 cm\n                    <jats:sup>2<\/jats:sup>\n                    ) shows an exceptional efficiency of 26.57% (certified 26.4%) along with enhanced thermal and operational stability. The strategy is also extended to large area devices, delivering efficiencies of 25.0% for a 1\u00a0cm\n                    <jats:sup>2<\/jats:sup>\n                    device and 22.9% for a 12.96\u00a0cm\n                    <jats:sup>2<\/jats:sup>\n                    minimodule. This study highlights the halogen role of interfacial small molecules in optimizing molecular packing and interfacial contact toward highly efficient PSCs with minimized energy loss and non\u2010radiative recombination.\n                  <\/jats:p>","DOI":"10.1002\/anie.202503008","type":"journal-article","created":{"date-parts":[[2025,4,21]],"date-time":"2025-04-21T06:40:51Z","timestamp":1745217651000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":50,"title":["Optimizing Molecular Packing and Interfacial Contact via Halogenated N\u2010Glycidyl Carbazole Small Molecules for Low Energy Loss and Highly Efficient Inverted Perovskite Solar Cells"],"prefix":"10.1002","volume":"64","author":[{"given":"Zhilu","family":"Xu","sequence":"first","affiliation":[{"name":"School of Chemical Engineering State Key Laboratory of Polymer Materials Engineering Engineering Research Center of Alternative Energy Materials &amp; Devices Ministry of Education Sichuan University  Chengdu 610065 P.R. 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