AI Article Synopsis

  • A two-step silica-encapsulation procedure increases both the optical efficiency and structural strength of TDBC, achieving a record fluorescence quantum yield of ∼98% at room temperature and a quick emissive lifetime of 234 ps.
  • * The silica coating, averaging 0.5-1 nm thick, maintains the optical properties of TDBC J-aggregates and allows for significant dilution without compromising integrity.
  • * This new silica TDBC J-aggregate structure serves as a powerful fluorophore system, a platform for integrating with other optical components, and a tool for studying exciton behaviors in a stable environment.

Article Abstract

We introduce a two-step silica-encapsulation procedure to optimize both the optical efficiency and structural robustness of 5,5',6,6'-tetrachloro-1,1'-diethyl-3,3'-di(4-sulfobutyl)-benzimidazolocarbocyanine (TDBC), a two-dimensional sheet-like J-aggregate. We report a fluorescence quantum yield of ∼98%, the highest quantum yield recorded for any J-aggregate structure at room temperature, and a fast, emissive lifetime of 234 ps. Silica, as an encapsulating matrix, provides optical transparency, chemical inertness, and robustness to dilution, while rigidifying the J-aggregate structure. Our in situ encapsulation process preserves the excitonic structure in TDBC J-aggregates, maintaining their light absorption and emission properties. The homogeneous silica coating has an average thickness of 0.5-1 nm around J-aggregate sheets. Silica encapsulation permits extensive dilutions of J-aggregates without significant disintegration into monomers. The narrow absorbance and emission line widths exhibit further narrowing upon cooling to 79 K, which is consistent with J-type coupling in the encapsulated aggregates. This silica TDBC J-aggregate construct signifies (1) a bright, fast, and robust fluorophore system, (2) a platform for further manipulation of J-aggregates as building blocks for integration with other optical materials and structures, and (3) a system for fundamental studies of exciton delocalization, transport, and emission dynamics within a rigid matrix.

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http://dx.doi.org/10.1021/acsnano.4c04732DOI Listing

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