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    Single-Molecule Fluorescence Spectroscopy of Phase-Separated 10,12-Pentacosadynoic Acid Films

    Year: 2021

    Journal: J. Phys. Chem. B, Volume 125, APR 22, page 3953–3962

    Authors: Yeboah, Alfred; Sowah-Kuma, David; Bu, Wei; Paige, Matthew F.

    Organizations: Natural Sciences and Engineering Research Council; Canadian Foundation for Innovation; University of Saskatchewan; Division of Chemistry (CHE), National Science Foundation [NSF/CHE-1834750]; Division of Materials Research (DMR), National Science Foundation [NSF/CHE-1834750]; U.S. DOE [DE-AC02-06CH11357]

    Phase-separated monolayers of 10,12-pentacosadiynoic acid and perfluorotetradecanoic acid can be photopolymerized to produce micrometer-sized, fluorescent polydiacetylene fibers at the air-solid interface. The photopolymer fibers were not uniformly fluorescent but rather showed a series of fluorescent spots along their lengths. The spots exhibited the classic properties of single-molecule fluorescence emission, including diffraction-limited size and fluorescence intermittency (on-off blinking). We have analyzed the fluorescence blinking dynamics of these spots using a variety of single-molecule analysis approaches, including fluorescence intensity histograms, autocorrelation analysis, as well as cross-correlation analysis as a function of distance between individual transition dipole moments, and propose a simple physical model for the fiber structure based on the observed blinking dynamics, in which the polymer fibers contain numerous structural defects. The model was supported by grazing incidence X-ray diffraction measurements of the mixed monolayer films at the air-water interface, in which it was observed that the presence of perfluorocarbon in the mixed monolayers significantly inhibited the ability of the 10,12-pentacosadiynoic acid to polymerize.
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