Super-resolution Imaging of Plasmonic Near-Fields: Overcoming Emitter Mislocalizations

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Abstract

Plasmonic nano-objects have shown great potential in enhancing applications like biological/chemical sensing, light harvesting and energy transfer, and optical/quantum computing. Therefore, an extensive effort has been vested in optimizing plasmonic systems and exploiting their field enhancement properties. Super-resolution imaging with quantum dots (QDs) is a promising method to probe plasmonic near-fields but is hindered by the distortion of the QD radiation pattern. Here, we investigate the interaction between QDs and "L-shaped"gold nanoantennas and demonstrate both theoretically and experimentally that this strong interaction can induce polarization-dependent modifications to the apparent QD emission intensity, polarization, and localization. Based on FDTD simulations and polarization-modulated single-molecule microscopy, we show that the displacement of the emitter's localization is due to the position-dependent interference between the emitter and the induced dipole, and can be up to 100 nm. Our results help pave a pathway for higher precision plasmonic near-field mapping and its underlying applications.

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Miao, Y., Boutelle, R. C., Blake, A., Chandrasekaran, V., Sheehan, C. J., Hollingsworth, J., … Weiss, S. (2022). Super-resolution Imaging of Plasmonic Near-Fields: Overcoming Emitter Mislocalizations. Journal of Physical Chemistry Letters, 13(20), 4520–4529. https://doi.org/10.1021/acs.jpclett.1c04123

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