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This study focuses on the competitive relaxation pathways after excitation to the lowest excited band of phenanthroline, that is, charge\u2010transfer (CT), and intramolecular benzene excimer formation, which govern its dual\u2010emission behavior. After excitation of the lowest excited band of dibenzophenanthroline, with \u03bb<jats:sub>exc\u00a0<\/jats:sub>=\u00a0500\u00a0nm DBP6 in DCM exhibits dominant excimer emission at 570\u00a0nm with a long\u2010lived fluorescence lifetime of 12\u00a0ns. This emission is attributed to stable \u03c0\u2010\u03c0 interactions between side phenyl rings. In contrast, excitation \u03bb<jats:sub>exc\u00a0<\/jats:sub>=\u00a0440\u00a0nm leads, in addition to excimer formation, also to weak S<jats:sub>1<\/jats:sub> emission at 480\u00a0nm (t\u00a0=\u00a00.34\u00a0ns). Higher\u2010energy excitation \u03bb<jats:sub>exc\u00a0<\/jats:sub>&lt;\u00a0370\u00a0nm reveals ultrafast CT state formation as an intermediate bridging S<jats:sub>1<\/jats:sub> depopulation and excimer generation. Solvent polarity\u2010dependent studies demonstrate a progressive red\u2010shift in S<jats:sub>1<\/jats:sub> emission (455\u00a0nm in toluene to 515\u00a0nm in ethanol) confirming CT state stabilization in polar environments. DFT simulations corroborate experimental results, predicting S<jats:sub>1<\/jats:sub> emission at 495\u00a0nm. By varying excitation wavelength and solvent polarity, DBP6's dual emission can be tuned, highlighting its potential for ratiometric sensing, stable organic light\u2010emitting diodes (OLEDs), and energy conversion systems. This work advances the understanding of nonlinear heteroacenes and provides a framework for designing optoelectronic materials with tailored excited\u2010state interactions.<\/jats:p>","DOI":"10.1002\/asia.202500658","type":"journal-article","created":{"date-parts":[[2025,6,20]],"date-time":"2025-06-20T04:10:33Z","timestamp":1750392633000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Competitive Relaxation Pathways of Dibenzophenanthroline Isomer Emission: Charge\u2010Transfer, Excimer Formation"],"prefix":"10.1002","volume":"20","author":[{"given":"Yichen","family":"Zhou","sequence":"first","affiliation":[{"name":"School of Light Industry and Chemical Engineering Dalian Polytechnic University  Dalian 116024 China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Junxiang","family":"Huang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Fine Chemicals Institute of Artificial Photosynthesis Dalian University of Technology  Dalian 116024 China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Animesh","family":"Ghosh","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Nanyang Technological University  Singapore 639798 Singapore"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Andrew C.","family":"Grimsdale","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Nanyang Technological University  Singapore 639798 Singapore"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Saran","family":"Long","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Fine Chemicals Institute of Artificial Photosynthesis Dalian University of Technology  Dalian 116024 China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Qi","family":"Tao","sequence":"additional","affiliation":[{"name":"School of Light Industry and 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