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However, significant non\u2010radiative carrier recombination under low\u2010light conditions has limited the full potential of perovskite\u2010based IPVs. To address this challenge, an integration of perylene diimide (PDI)\u2010based sulfobetaines as cathode interlayers (CILs) is proposed and the impact of varying alkyl chain length (from 1,2\u2010ethylene to 1,5\u2010pentylene) between the cationic and the anionic moieties is examined. The respective four PDI materials are synthesized almost qualitatively using a one\u2010step microwave\u2010assisted process. All of them show adequate thermal stability and energy levels suitable for the desired application as CILs. Moreover, their degradation temperature, LUMO level, conductivity, and performance in model devices are found to change positively along with the alkyl chain length increase. Among the tested derivatives, the compound equipped with the longest alkyl chain (PDI\u2010C5\u2010S3) stands out for its superior electrical conductivity and enhanced ability to lower the silver cathode work function. When incorporated into Cs<jats:sub>0.18<\/jats:sub>FA<jats:sub>0.82<\/jats:sub>Pb(I<jats:sub>0.8<\/jats:sub>Br<jats:sub>0.2<\/jats:sub>)\u2010based wide\u2010bandgap perovskite solar cells (PSCs), the PDI\u2010C5\u2010S3 interlayer lead to an outstanding power conversion efficiency (PCE) of 19.04% under one\u2010sun illumination and a remarkable 40.72% under 3000K LED (1000 lux) conditions.<\/jats:p>","DOI":"10.1002\/smll.202411623","type":"journal-article","created":{"date-parts":[[2025,3,13]],"date-time":"2025-03-13T04:44:52Z","timestamp":1741841092000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Highly Efficient Indoor Perovskite Solar Cells with 40% Efficiency Using Perylene Diimide\u2010Based Zwitterionic Cathode Interlayers"],"prefix":"10.1002","volume":"21","author":[{"given":"Bartosz","family":"Orwat","sequence":"first","affiliation":[{"name":"Department of Molecular Physics Faculty of Chemistry Lodz 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