In the present work, bilayered hybrids obtained by hydrosilylation of polysiloxane with carbazolyl moieties (Sil‐Cz) and polyfluorene (Sil‐PFO) had their photophysical behavior, morphological characteristics and interaction properties studied for applications in electroluminescent devices. Fluorescence spectra of the Sil‐Cz did not show emission in the excimer/aggregate region (from 400 to 500 nm). This is an unexpected behavior since most of the carbazole‐based materials present excimer and aggregation. Nonetheless, this unusual observation was also predicted by geometry optimization calculations. Fluorescence spectra were taken for both compounds separately and for the bilayered system show some evidence of interaction between carbazolyl and polyfluorene moieties, giving rise to the supposition that the can form a system with tunable luminescent properties.
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