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Here, we introduce a pump\u2010probe\u2010only, solvent\u2010polarity\u2010based strategy to resolve this problem using 1,8\u2010naphthalimide D\u2010A chromophores. In nonpolar n\u2010hexane, resonant LE\u2010CT coupling generates persistent coherent beating, whereas in polar dichloromethane, the CT state is stabilized, the LE\u2010CT gap widens, and vibronic coherence is quenched while vibrational oscillations remain comparatively robust. This establishes a practical diagnostic for identifying LE\u2010CT vibronic mixing without recourse to temperature variation or two\u2010dimensional spectroscopy. Beyond coherence assignment, the same LE\u2010CT coupling explains intensity borrowing and the appearance of CT absorption even in near\u2010orthogonal geometries, providing a route to estimate the effective CT transition dipole and to rationalize enhanced optical absorption. Finally, we show unprecedented polarity\u2010controlled switching between TADF and triplet\u2013triplet annihilation (TTA) in a single deep\u2010blue emitter, thereby linking coherence physics, LE\u2010CT electronic structure, and triplet harvesting into a unified framework for designing polarity\u2010robust optoelectronic materials.<\/jats:p>","DOI":"10.1002\/smsc.70387","type":"journal-article","created":{"date-parts":[[2026,8,21]],"date-time":"2026-08-21T14:22:55Z","timestamp":1787322175000},"source":"Crossref","is-referenced-by-count":0,"title":["Solvent Polarity as a Diagnostic for Vibronic\/Vibrational Coherences Distinction in an Efficient TADF\u2010TTA Switchable Emitter"],"prefix":"10.1002","volume":"6","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-1783-1586","authenticated-orcid":false,"given":"Ajeet K.","family":"Singh","sequence":"first","affiliation":[{"name":"Department of Chemistry Birla Institute of Technology and Science Pilani Campus  Pilani Rajasthan 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