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In this study, steady\u2010state and transient absorption spectroscopy are employed to disentangle the spectral signatures and excited\u2010state dynamics of interacting and noninteracting Y6 in solution and thin films. By controlling aggregation in dilute solution, we identify localized Frenkel\u2010type excitons (LE) on noninteracting Y6 and aggregate excitons (AE) on intermolecular interacting Y6. The AEs exhibit strongly fluence\u2010dependent lifetimes (30\u2013200\u00a0ps) governed by singlet\u2013singlet annihilation, whereas localized excitons decay monoexponentially on a nanosecond timescale. Furthermore, long\u2010lived polaronic states are observed to form on aggregated Y6 within tens of picoseconds and persist into the nanosecond regime. Comparison with thin\u2010film measurements reveals similar processes with an additional ultrafast energy transfer from noninteracting chromophores to aggregated domains. These results establish a consistent framework for assigning transient absorption features in Y6 and suggest that, in neat films of Y6, the pairwise formation of polarons arises from an Onsager\u2010like autoionization process of delocalized excitons in domains of interacting Y6 with moderate yield. This provides central insight into charge\u2010generation mechanisms in Y6\u2010based photovoltaic systems.<\/jats:p>","DOI":"10.1002\/adma.75428","type":"journal-article","created":{"date-parts":[[2026,10,19]],"date-time":"2026-10-19T03:22:52Z","timestamp":1792380172000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Disentangling Polaron Formation Pathways in Y6 by Probing Noninteracting and Interacting Chromophores via Transient Absorption Spectroscopy"],"prefix":"10.1002","author":[{"given":"Daniel","family":"Kroh","sequence":"first","affiliation":[{"name":"Soft Matter Optoelectronics Experimentalphysik II Bayreuth Institute of Macromolecular Research (BIMF) Bavarian Polymer Institute (BPI) and Bayreuth Centre For Material Science and Engineering (BayMAT) University of Bayreuth  Bayreuth Germany"},{"name":"School of Chemistry University of Melbourne  Parkville Victoria Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-9349-8703","authenticated-orcid":false,"given":"Xinyue","family":"Xu","sequence":"additional","affiliation":[{"name":"School of Chemistry University of Melbourne  Parkville Victoria Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4453-9713","authenticated-orcid":false,"given":"Trevor A.","family":"Smith","sequence":"additional","affiliation":[{"name":"School of Chemistry University of Melbourne  Parkville Victoria Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5029-4420","authenticated-orcid":false,"given":"Anna","family":"K\u00f6hler","sequence":"additional","affiliation":[{"name":"Soft Matter Optoelectronics Experimentalphysik II Bayreuth Institute of Macromolecular Research (BIMF) Bavarian Polymer Institute (BPI) and Bayreuth Centre For Material Science and Engineering (BayMAT) University of Bayreuth  Bayreuth Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,10,18]]},"reference":[{"key":"e_1_2_11_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2019.01.004"},{"key":"e_1_2_11_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsenergylett.0c02384"},{"key":"e_1_2_11_4_1","doi-asserted-by":"crossref","first-page":"2029","DOI":"10.1002\/nano.202100036","article-title":"Recent Progress of Y\u2010Series Electron Acceptors for Organic Solar Cells","volume":"2","author":"Lu B.","year":"2021","journal-title":"Nano Select"},{"key":"e_1_2_11_5_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1TA10707K"},{"key":"e_1_2_11_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010023\u201037526\u20105"},{"key":"e_1_2_11_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202000975"},{"key":"e_1_2_11_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.1c00742"},{"key":"e_1_2_11_9_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2018.11.023"},{"key":"e_1_2_11_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202103422"},{"key":"e_1_2_11_11_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010020\u201019853\u2010z"},{"key":"e_1_2_11_12_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010020\u201017867\u20101"},{"key":"e_1_2_11_13_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2022.01.006"},{"key":"e_1_2_11_14_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.mtadv.2021.100154"},{"key":"e_1_2_11_15_1","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202514004"},{"key":"e_1_2_11_16_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560\u2010024\u201001678\u20105"},{"key":"e_1_2_11_17_1","doi-asserted-by":"publisher","DOI":"10.1039\/D4EE03815K"},{"key":"e_1_2_11_18_1","doi-asserted-by":"publisher","DOI":"10.1039\/D3TA05177C"},{"key":"e_1_2_11_19_1","doi-asserted-by":"publisher","DOI":"10.3390\/ijms241914753"},{"key":"e_1_2_11_20_1","doi-asserted-by":"crossref","first-page":"591","DOI":"10.1002\/sus2.82","article-title":"Molecular Engineering of Y\u2010Series Acceptors for Nonfullerene Organic Solar Cells","volume":"2","author":"He Q.","year":"2022","journal-title":"SusMat"},{"key":"e_1_2_11_21_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010024\u201047052\u20107"},{"key":"e_1_2_11_22_1","doi-asserted-by":"publisher","DOI":"10.1063\/5.0138748"},{"key":"e_1_2_11_23_1","doi-asserted-by":"crossref","DOI":"10.1002\/adfm.202419236","article-title":"Analyzing Electronic Excitations and Exciton Binding Energies in Y6 Films","volume":"36","author":"Akram S. 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