Quantum yield and excitation rate of single molecules close to metallic nanostructures

Phil Holzmeister, Enrico Pibiri, Jürgen J. Schmied, Tapasi Sen, Guillermo P. Acuna () and Philip Tinnefeld ()
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Phil Holzmeister: NanoBioSciences Group, Institute for Physical and Theoretical Chemistry and Braunschweig Integrated Centre of Systems Biology (BRICS), and Laboratory for Emerging Nanometrology (LENA), Braunschweig University of Technology
Enrico Pibiri: NanoBioSciences Group, Institute for Physical and Theoretical Chemistry and Braunschweig Integrated Centre of Systems Biology (BRICS), and Laboratory for Emerging Nanometrology (LENA), Braunschweig University of Technology
Jürgen J. Schmied: NanoBioSciences Group, Institute for Physical and Theoretical Chemistry and Braunschweig Integrated Centre of Systems Biology (BRICS), and Laboratory for Emerging Nanometrology (LENA), Braunschweig University of Technology
Tapasi Sen: NanoBioSciences Group, Institute for Physical and Theoretical Chemistry and Braunschweig Integrated Centre of Systems Biology (BRICS), and Laboratory for Emerging Nanometrology (LENA), Braunschweig University of Technology
Guillermo P. Acuna: NanoBioSciences Group, Institute for Physical and Theoretical Chemistry and Braunschweig Integrated Centre of Systems Biology (BRICS), and Laboratory for Emerging Nanometrology (LENA), Braunschweig University of Technology
Philip Tinnefeld: NanoBioSciences Group, Institute for Physical and Theoretical Chemistry and Braunschweig Integrated Centre of Systems Biology (BRICS), and Laboratory for Emerging Nanometrology (LENA), Braunschweig University of Technology

Nature Communications, 2014, vol. 5, issue 1, 1-9

Abstract: Abstract The interaction of dyes and metallic nanostructures strongly affects the fluorescence and can lead to significant fluorescence enhancement at plasmonic hot spots, but also to quenching. Here we present a method to distinguish the individual contributions to the changes of the excitation, radiative and non-radiative rate and use this information to determine the quantum yields for single molecules. The method is validated by precisely placing single fluorescent dyes with respect to gold nanoparticles as well as with respect to the excitation polarization using DNA origami nanostructures. Following validation, measurements in zeromode waveguides reveal that suppression of the radiative rate and enhancement of the non-radiative rate lead to a reduced quantum yield. Because the method exploits the intrinsic blinking of dyes, it can generally be applied to fluorescence measurements in arbitrary nanophotonic environments.

Date: 2014
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DOI: 10.1038/ncomms6356

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