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Harrison J. Goldwyn , Kevin C. Smith , Jacob A. Busche , and David J. Masiello*Roxy Flat Klogs USA US Women's 6 5 Barely
Department of Chemistry, University of Washington , Seattle , Washington 98195 , United States
Department of Physics, University of Washington, Seattle , Washington 98195 , United States
ACS Photonics, 2018, 5 (8), pp 3141–3151
DOI: 10.1021/acsphotonics.8b00372
Publication Date (Web): May 9, 2018
Copyright © 2018 American Chemical Society


Mislocalization is a quantitative measure of the inability to locate the positions of individual molecular emitters in plasmon-enhanced super-resolution fluorescence microscopy. It is due to an unfortunate side-effect that scrambles the spatial profile of a molecule’s fluorescence signal when plasmonic nanoantennas are introduced to boost that signal. In this article, we present an understanding of the mislocalization problem in plasmon-enhanced super-resolution fluorescence microscopy based upon a simple and intuitive theoretical model. In particular, we derive an analytic expression for mislocalization and demonstrate explicitly how it depends upon both the macroscopic interference of the coherent emission from molecular and plasmonic emitters and the microscopic dynamics of the coupled system. To derive this expression, we draw upon an analogy to the Fano interference problem and show that the spatial asymmetry in the intensity profile can be encapsulated into a single effective parameter that depends rigorously upon basic system properties. We further elucidate the causes of mislocalization within the context of hybridization between molecular and plasmonic emitters and show analytically how the localization error depends upon the relative separation, orientation, detuning, and polarizability of the emitters. Lastly, we derive a new model-based form of the plasmon-enhanced single-molecule fluorescence image for specified molecular dipole orientations and demonstrate that it significantly outperforms standard Gaussian fitting in locating the position of the molecule.

The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsphotonics.8b00372.

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Received 22 March 2018
Published online 9 May 2018
Published in print 15 August 2018
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