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

Yuting Miao; Robert C. Boutelle; Anastasia Blake; Vigneshwaran Chandrasekaran; Chris J. Sheehan; Jennifer Hollingsworth; Daniel Neuhauser; Shimon Weiss

doi:10.1021/acs.jpclett.1c04123

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

Yuting Miao, Robert C. Boutelle, Anastasia Blake, Vigneshwaran Chandrasekaran, Chris J. Sheehan, Jennifer Hollingsworth, Daniel Neuhauser, Shimon Weiss

Department of Physics - at Bar-Ilan University

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

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.

Original language	English
Pages (from-to)	4520-4529
Number of pages	10
Journal	Journal of Physical Chemistry Letters
Volume	13
Issue number	20
DOIs	https://doi.org/10.1021/acs.jpclett.1c04123
State	Published - 26 May 2022

Bibliographical note

Publisher Copyright:
© 2022 American Chemical Society.

Funding

This project is supported by National Science Foundation (NSF) Grant 1808766 and Center for Integrated Nanotechnologies (CINT) User Project 2020AC0003. CINT is an Office of Science (OS) Nanoscale Science Research Center (NSRC) and User Facility operated for the U.S. Department of Energy (DOE) by Los Alamos National Laboratory (LAN L; Contract No. DE-AC52-06NA25396) and Sandia National Laboratories (Contract No. DE-NA-0003525). The sample fabrication, optical measurement, and simulations are carried out at University of California, Los Angeles (UCLA). DPN experiments are conducted at Los Alamos National Lab. A.B. and C.J.S. are CINT-funded technical specialists. V.C. is supported by the CINT postdoctoral funding.

Funders	Funder number
Nanoscale Science Research Center
National Science Foundation	1808766
U.S. Department of Energy
Office of Science
Sandia National Laboratories	DE-NA-0003525
University of California, Los Angeles
Los Alamos National Laboratory	DE-AC52-06NA25396
Center for Integrated Nanotechnologies	2020AC0003

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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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AU - Chandrasekaran, Vigneshwaran

AU - Sheehan, Chris J.

AU - Hollingsworth, Jennifer

AU - Neuhauser, Daniel

AU - Weiss, Shimon

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

Abstract

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