Sub-nanometre control of the coherent interaction between a single molecule and a plasmonic nanocavity

Yao Zhang, Qiu-Shi Meng, Li Zhang, Yang Luo, Yun-Jie Yu, Ben Yang, Yang Zhang, Ruben Esteban, Javier Aizpurua (), Yi Luo, Jin-Long Yang, Zhen-Chao Dong () and J G Hou ()
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Yao Zhang: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China
Qiu-Shi Meng: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China
Li Zhang: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China
Yang Luo: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China
Yun-Jie Yu: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China
Ben Yang: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China
Yang Zhang: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China
Ruben Esteban: Donostia International Physics Center (DIPC), Paseo Manuel de Lardizabal 4
Javier Aizpurua: Materials Physics Center (CSIC-UPV/EHU), Paseo Manuel de Lardizabal 5
Yi Luo: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China
Jin-Long Yang: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China
Zhen-Chao Dong: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China
J G Hou: Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China

Nature Communications, 2017, vol. 8, issue 1, 1-7

Abstract: Abstract The coherent interaction between quantum emitters and photonic modes in cavities underlies many of the current strategies aiming at generating and controlling photonic quantum states. A plasmonic nanocavity provides a powerful solution for reducing the effective mode volumes down to nanometre scale, but spatial control at the atomic scale of the coupling with a single molecular emitter is challenging. Here we demonstrate sub-nanometre spatial control over the coherent coupling between a single molecule and a plasmonic nanocavity in close proximity by monitoring the evolution of Fano lineshapes and photonic Lamb shifts in tunnelling electron-induced luminescence spectra. The evolution of the Fano dips allows the determination of the effective interaction distance of ∼1 nm, coupling strengths reaching ∼15 meV and a giant self-interaction induced photonic Lamb shift of up to ∼3 meV. These results open new pathways to control quantum interference and field–matter interaction at the nanoscale.

Date: 2017
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DOI: 10.1038/ncomms15225

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