Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 98, Issue 26, Pages 14769-14772Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.251555298
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Fluorescence superquenching is investigated for polyelectrolytes consisting of cyanine dye pendant polylysines ranging in number of polymer repeat units (N-PRU) from 1 to 900, both in solution and after adsorption onto silica nanoparticles. As N-PRU increases, the absorption and fluorescence evolve from monomer spectra to red-shifted features indicative of molecular J aggregates. In solution, the superquenching sensitivity toward an anionic electron acceptor increases by more than a millionfold over the N-PRU range from I to 900. The dramatic increase is attributed to enhanced equilibrium constants for binding the quenchers, and the amplified quenching of a delocalized exciton of approximate to 100 polymer repeat units. The self-assembly of monomer onto silica and clay nanoparticles leads to formation of J aggregates, and surf ace-activated superquenching enhanced 10,000x over the monomer in solution, indicating the formation of self-assembled polymers on the nanoparticle surface. Utilization of these self-assembled polymers as high-sensitivity biosensors is demonstrated.
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