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A strategy for the design of highly emissive organic phosphors is still hard to predict, thus impeding the development of new functional materials with the desired optical properties. Herein, we analyze a family of alkyl and aryl\u2010substituted persulfurated benzenes, the latter representing a class of organic solid\u2010state triplet emitters able to show very high emission quantum yield at room temperature. In this work, we correlate structural parameters with the photophysical properties observed in different experimental conditions (diluted solution, crystalline and amorphous phase at RT and low temperature). Our results, corroborated by a detailed computational analysis, indicate a close relationship between the luminescence properties and i) the nature of the substituents on the persulfurated core, ii) the adopted conformations in the solid state, both in crystalline and amorphous phases. These factors contribute to characterize the lowest\u2010energy lying excited\u2010state, its deactivation pathways, the phosphorescence lifetime and quantum yield. These findings provide a useful roadmap for the development of highly performing purely organic solid\u2010state emitters based on the persulfurated benzene platform.<\/jats:p>","DOI":"10.1002\/chem.202401768","type":"journal-article","created":{"date-parts":[[2024,5,31]],"date-time":"2024-05-31T07:06:22Z","timestamp":1717139182000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Unravelling the Role of Structural Factors in the Luminescence Properties of Persulfurated Benzenes"],"prefix":"10.1002","volume":"30","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1080-0530","authenticated-orcid":false,"given":"Andrea","family":"Fermi","sequence":"first","affiliation":[{"name":"Dipartimento di Chimica \u201cGiacomo Ciamician\u201d Alma Mater Studiorum \u2013 Universit\u00e0 di Bologna  Via Selmi 2 40126 Bologna 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