Abstract
Understanding the parameters that control the intermolecular interactions of chromophores encapsulated within nanoparticles is of fundamental importance to various fields of nanoscience. Employing single-molecule time and spectral domains, we studied a red-absorbing hemicyanine analogue (DY-630) covalently encapsulated in the core of ∼20 and ∼30 nm core–shell silica nanoparticles. We find that on average 4 and 7 dyes are encapsulated within these particles, respectively. Steady state and fluorescence correlation spectroscopy show unusually strong enhancements (up to 16 times) in the relative fluorescence efficiency of the nanoparticles as compared to the free dye in aqueous solution. This increase is explained in terms of restriction of the trans–cis isomerization process due to the more rigid local environment provided by the silica, and protection from the solute–solvent interaction, while preserving the spectral characteristics of the constituent dye. Single molecule measurements reveal that the majori...
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