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Herein, the photoexcited\u2010state dynamics of homo\u2010sorted \u03c0\u2010stacked aggregates of a naphthalenemonoimide and perylene\u2010based acceptor\u2010donor (<jats:bold>NI\u2010Pe<\/jats:bold>) system and a fork\u2010shaped acceptor\u2010bisdonor (<jats:bold>NI\u2010Pe<jats:sub>2<\/jats:sub><\/jats:bold>) system possessing integrally stacked peri\u2010substituted donors was examined. Femtosecond transient absorption (fsTA) spectra of <jats:bold>NI\u2010Pe<\/jats:bold> monomer recorded in chloroform displayed spectroscopic signatures of the singlet state of Pe; <jats:sup>1<\/jats:sup>Pe*, the charge\u2010separated state; NI<jats:sup>\u2212<\/jats:sup>\u22c5\u2010Pe<jats:sup>+<\/jats:sup>\u22c5, and the triplet state of Pe; <jats:sup>3<\/jats:sup>Pe*. The examination of ultrafast excited\u2010state processes of <jats:bold>NI\u2010Pe<\/jats:bold> aggregate in chloroform revealed faster charge recombination (\n=1.75\u2005ns) than the corresponding monomer (\n=2.46\u2005ns) which was followed by observation of a broad structureless band attributed to an excimer\u2010like state. The fork\u2010shaped <jats:bold>NI\u2010Pe<jats:sub>2<\/jats:sub><\/jats:bold> displayed characteristic spectroscopic features of the NI radical anion (\u03bb<jats:sub>max<\/jats:sub>~450\u2005nm) and perylene dimer radical cation (\u03bb<jats:sub>max<\/jats:sub>~520\u2005nm) upon photoexcitation in non\u2010polar toluene solvent in the nanosecond transient absorption (nsTA) spectroscopy. The investigation highlights the significance of intrinsic close\u2010stacked arrangement of donors in ensuring a long\u2010lived photoinduced charge\u2010separated state (\n=1.35\u2005\u03bcs) in non\u2010polar solvents via delocalization of radical cation between the donors.<\/jats:p>","DOI":"10.1002\/chem.202401969","type":"journal-article","created":{"date-parts":[[2024,7,3]],"date-time":"2024-07-03T02:39:39Z","timestamp":1719974379000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Excited\u2010State Dynamics in Segregated Donor\u2010Acceptor Stacks Versus a Peri\u2010Bisdonor\u2010Acceptor System"],"prefix":"10.1002","volume":"30","author":[{"given":"Remya","family":"Ramakrishnan","sequence":"first","affiliation":[{"name":"School of Chemistry Indian Institute of Science Education, Research Thiruvananthapuram (IISER TVM)  Maruthamala P.O. 695551 Vithura, Thiruvananthapuram, Kerala India"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Meera","family":"Madhu","sequence":"additional","affiliation":[{"name":"School of Chemistry Indian Institute of Science Education, Research Thiruvananthapuram (IISER TVM)  Maruthamala P.O. 695551 Vithura, Thiruvananthapuram, Kerala India"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Hruidya C.","family":"Babu","sequence":"additional","affiliation":[{"name":"School of Chemistry Indian Institute of Science Education, Research Thiruvananthapuram (IISER TVM)  Maruthamala P.O. 695551 Vithura, Thiruvananthapuram, Kerala India"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Ebin","family":"Sebastian","sequence":"additional","affiliation":[{"name":"School of Chemistry Indian Institute of Science Education, Research Thiruvananthapuram (IISER TVM)  Maruthamala P.O. 695551 Vithura, Thiruvananthapuram, Kerala India"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3237-6235","authenticated-orcid":false,"given":"Mahesh","family":"Hariharan","sequence":"additional","affiliation":[{"name":"School of Chemistry Indian Institute of Science Education, Research Thiruvananthapuram (IISER TVM)  Maruthamala P.O. 695551 Vithura, Thiruvananthapuram, Kerala India"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"311","published-online":{"date-parts":[[2024,8,20]]},"reference":[{"doi-asserted-by":"publisher","key":"e_1_2_8_1_1","DOI":"10.1016\/j.chphma.2022.05.002"},{"key":"e_1_2_8_2_1","volume":"28","author":"Wang C.","year":"2022","journal-title":"Chem.Eur. 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