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In this work, the top surface treatment of mixed tin\u2013lead (\u22481.26\u00a0eV) halide perovskite films for p\u2013i\u2013n solar cells is studied. Charge extraction is promoted by treating the perovskite surface with piperazine. This compound reacts with the organic cations at the perovskite surface, modifying the surface structure and tuning the interfacial energy level alignment. In addition, the combined treatment with C<jats:sub>60<\/jats:sub> pyrrolidine tris\u2010acid (CPTA) reduces hysteresis and leads to efficiencies up to 22.7%, with open\u2010circuit voltage values reaching 0.90\u00a0V, \u224892% of the radiative limit for the bandgap of this material. The modified cells also show superior stability, with unencapsulated cells retaining 96% of their initial efficiency after &gt;2000 h of storage in N<jats:sub>2<\/jats:sub> and encapsulated cells retaining 90% efficiency after &gt;450 h of storage in air. Intriguingly, CPTA preferentially binds to Sn<jats:sup>2+<\/jats:sup> sites at film surface over Pb<jats:sup>2+<\/jats:sup> due to the energetically favored exposure of the former, according to first\u2010principles calculations. This work provides new insights into the surface chemistry of perovskite films in terms of their structural, electronic, and defect characteristics and this knowledge is used to fabricate state\u2010of\u2010the\u2010art solar cells.<\/jats:p>","DOI":"10.1002\/adma.202208320","type":"journal-article","created":{"date-parts":[[2022,12,8]],"date-time":"2022-12-08T18:39:51Z","timestamp":1670524791000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":95,"title":["Synergistic Surface Modification of Tin\u2013Lead Perovskite Solar Cells"],"prefix":"10.1002","volume":"35","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1312-075X","authenticated-orcid":false,"given":"Shuaifeng","family":"Hu","sequence":"first","affiliation":[{"name":"Institute for Chemical Research Kyoto University  Gokasho Uji Kyoto 611\u20100011 Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8088-6141","authenticated-orcid":false,"given":"Pei","family":"Zhao","sequence":"additional","affiliation":[{"name":"Research Center for Computational Science Institute for Molecular Science  Okazaki 444\u20138585 Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2493-2817","authenticated-orcid":false,"given":"Kyohei","family":"Nakano","sequence":"additional","affiliation":[{"name":"RIKEN Center for Emergent Matter Science (CEMS)  Wako Saitama 351\u20100198 Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4980-7940","authenticated-orcid":false,"given":"Robert D. 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