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Single Molecule Nonlinearity in a Plasmonic Waveguide

Cite this: Nano Lett. 2020, 20, 3, 2152–2156
Publication Date (Web):February 20, 2020
Copyright © 2020 American Chemical Society

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    Abstract Image

    Plasmonic waveguides offer the unique possibility to confine light far below the diffraction limit. Past room temperature experiments focused on efficient generation of single waveguide plasmons by a quantum emitter. However, only the simultaneous interaction of the emitter with multiple plasmonic fields would lead to functionality in a plasmonic circuit. Here, we demonstrate the nonlinear optical interaction of a single molecule and propagating plasmons. An individual terrylene diimide (TDI) molecule is placed in the nanogap between two single-crystalline silver nanowires. A visible wavelength pump pulse and a red-shifted depletion pulse travel along the waveguide, leading to stimulated emission depletion (STED) in the observed fluorescence. The efficiency increases by up to a factor of 50 compared to far-field excitation. Our study thus demonstrates remote nonlinear four-wave mixing at a single molecule with propagating plasmons. It paves the way toward functional quantum plasmonic circuits and improved nonlinear single-molecule spectroscopy.

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    • Sample fabrication; optical setup; pump and depletion spot size; depletion statistics of TDI; lifetime histogram of TDI; quantifying the background emission; propagation of the depletion pulses; propagation loss with PMMA cover; supplementary note 1: numerical simulations; supplementary note 2: model for fluorescence suppression (PDF)

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    Cited By

    This article is cited by 15 publications.

    1. Michael Seidel, Yuhui Yang, Thorsten Schumacher, Yongheng Huo, Saimon Filipe Covre da Silva, Sven Rodt, Armando Rastelli, Stephan Reitzenstein, Markus Lippitz. Intermediate Field Coupling of Single Epitaxial Quantum Dots to Plasmonic Waveguides. Nano Letters 2023, 23 (22) , 10532-10537.
    2. Daniel Fersch, Pavel Malý, Jessica Rühe, Victor Lisinetskii, Matthias Hensen, Frank Würthner, Tobias Brixner. Single-Molecule Ultrafast Fluorescence-Detected Pump–Probe Microscopy. The Journal of Physical Chemistry Letters 2023, 14 (21) , 4923-4932.
    3. Maximilian Ochs, Luka Zurak, Enno Krauss, Jessica Meier, Monika Emmerling, René Kullock, Bert Hecht. Nanoscale Electrical Excitation of Distinct Modes in Plasmonic Waveguides. Nano Letters 2021, 21 (10) , 4225-4230.
    4. Vladimir Smirnov, Sven Stephan, Michael Westphal, Daniel Emmrich, André Beyer, Armin Gölzhäuser, Christoph Lienau, Martin Silies. Transmitting Surface Plasmon Polaritons across Nanometer-Sized Gaps by Optical near-Field Coupling. ACS Photonics 2021, 8 (3) , 832-840.
    5. Nicolò Maccaferri, Sophie Meuret, Nikolay Kornienko, Deep Jariwala. Speeding up Nanoscience and Nanotechnology with Ultrafast Plasmonics. Nano Letters 2020, 20 (8) , 5593-5596.
    6. Nasir Alfaraj, Charles Chih-Chin Lin, Sherif Nasif, Swati Rajput, Amr S. Helmy. Facile integration of electro-optic SiO<sub>2</sub>/ITO heterointerfaces in MIS structures for CMOS-compatible plasmonic waveguide modulation. Light: Advanced Manufacturing 2023, 4 (4) , 1.
    7. Farooq Abdulghafoor Khaleel, Shelan Khasro Tawfeeq. The modeling techniques of the second‐order correlation function g (2) ( τ ) for a quantum emitter. International Journal of Numerical Modelling: Electronic Networks, Devices and Fields 2022, 35 (5)
    8. Lokendra Singh, Prakash Pareek, Bahija Siddiqui, Eswara Prasad Konakalla. Investigation of Sensing Ability of Double-Slot Hybrid Plasmonic Waveguide for Liquid Analyte. 2022, 435-440.
    9. Yinhui Kan. On-Chip Control Excitations of Quantum Emitters in Hybrid Nanocircuits. 2022, 101-111.
    10. C.K. Jiang, J.H. Li, Z.H. Han, Y. Ma, Y.Q. Ma. Coupling of plasmon excited by single quantum emitters incorporated with metal nanoapertures. Optik 2022, 250 , 168323.
    11. Christian Schörner, Markus Lippitz. High-Q plasmonic nanowire-on-mirror resonators by atomically smooth single-crystalline silver flakes. The Journal of Chemical Physics 2021, 155 (23)
    12. Hong Wei, Xiaohong Yan, Yijie Niu, Qiang Li, Zhili Jia, Hongxing Xu. Plasmon–Exciton Interactions: Spontaneous Emission and Strong Coupling. Advanced Functional Materials 2021, 31 (51)
    13. Shailesh Kumar, Sergey I. Bozhevolnyi. Single Photon Emitters Coupled to Plasmonic Waveguides: A Review. Advanced Quantum Technologies 2021, 4 (10)
    14. Alessandro Tuniz. Nanoscale nonlinear plasmonics in photonic waveguides and circuits. La Rivista del Nuovo Cimento 2021, 44 (4) , 193-249.
    15. Yinhui Kan, Shailesh Kumar, Fei Ding, Changying Zhao, Sergey I. Bozhevolnyi. Spin–Orbit Controlled Excitation of Quantum Emitters in Hybrid Plasmonic Nanocircuits. Advanced Optical Materials 2020, 8 (21)

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