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Squaraines (SQs) could be a candidate for dopant\u2010free HTMs as they are natural passivators for perovskites. One major limitation of SQs is their relatively low hole mobility. Herein we demonstrate that polymerizing SQs into pseudo two dimensional (2D) p\u2013\u03c0 conjugated polymers could overcome this problem. By rationally using N,N\u2010diarylanilinosquaraines as the comonomers, the resulting polysquaraine HTMs not only exhibit suitable energy levels and efficient passivation effects, but also achieve very high hole mobility close to 0.01\u2005cm<jats:sup>\u22122<\/jats:sup>\u2009V<jats:sup>\u22121<\/jats:sup>\u2009s<jats:sup>\u22121<\/jats:sup>. Thus as dopant\u2010free HTMs for \u03b1\u2010CsPbI<jats:sub>2<\/jats:sub>Br\u2010based all\u2010inorganic PVSCs, the best PCE reached is 15.5\u2009%, outperforming those of the doped\u2010Spiro\u2010OMeTAD (14.4\u2009%) based control devices and among the best for all\u2010inorganic PVSCs.<\/jats:p>","DOI":"10.1002\/anie.201907331","type":"journal-article","created":{"date-parts":[[2019,9,27]],"date-time":"2019-09-27T10:48:32Z","timestamp":1569581312000},"page":"17724-17730","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":131,"title":["Dopant\u2010Free Squaraine\u2010Based Polymeric Hole\u2010Transporting Materials with Comprehensive Passivation Effects for Efficient All\u2010Inorganic Perovskite Solar Cells"],"prefix":"10.1002","volume":"58","author":[{"given":"Qi","family":"Xiao","sequence":"first","affiliation":[{"name":"Key Laboratory for Material Chemistry of Energy Conversion and Storage Ministry of Education School of Chemistry and Chemical Engineering Huazhong University of Science and Technology  Wuhan 430074 P. 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