Bright and Fast Emission from Robust Supramolecular J-Aggregate Nanostructures through Silica-Encapsulation
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Author(s)
Thanippuli Arachchi, Dimuthu H
Barotov, Ulugbek
Perkinson, Collin F
Šverko, Tara
Kaplan, Alexander EK
Bawendi, Moungi G
Date Issued
July 24, 2024
Journal
ACS Nano
Publisher
American Chemical Society
Citation
Bright and Fast Emission from Robust Supramolecular J-Aggregate Nanostructures through Silica-Encapsulation
Dimuthu H. Thanippuli Arachchi, Ulugbek Barotov, Collin F. Perkinson, Tara Šverko, Alexander E. K. Kaplan, and Moungi G. Bawendi. ACS Nano 2024 18 (31), 20422-20434.
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Author's final manuscript
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.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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DOI of Published Version
10.1021/acsnano.4c04732
