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Herein, a full investigation of the optical properties and first‐principles calculations of a large series of original 2‐(2′‐hydroxybenzofuran)benzazole (HBBX) dyes is described. The electronic substitution on the π‐conjugated core of the fluorophores and the nature of the heteroatom (O, S, N) was varied extensively to assess the necessary parameters to trigger a partial frustration of the excited‐state...
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