Quantum electrodynamics at room temperature coupling a single vibrating molecule with a plasmonic nanocavity

Oluwafemi S. Ojambati, Rohit Chikkaraddy, William D. Deacon, Matthew Horton, Dean Kos, Vladimir A. Turek, Ulrich F. Keyser and Jeremy J. Baumberg ()
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Oluwafemi S. Ojambati: University of Cambridge
Rohit Chikkaraddy: University of Cambridge
William D. Deacon: University of Cambridge
Matthew Horton: University of Cambridge
Dean Kos: University of Cambridge
Vladimir A. Turek: University of Cambridge
Ulrich F. Keyser: University of Cambridge
Jeremy J. Baumberg: University of Cambridge

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: Abstract Interactions between a single emitter and cavity provide the archetypical system for fundamental quantum electrodynamics. Here we show that a single molecule of Atto647 aligned using DNA origami interacts coherently with a sub-wavelength plasmonic nanocavity, approaching the cooperative regime even at room temperature. Power-dependent pulsed excitation reveals Rabi oscillations, arising from the coupling of the oscillating electric field between the ground and excited states. The observed single-molecule fluorescent emission is split into two modes resulting from anti-crossing with the plasmonic mode, indicating the molecule is strongly coupled to the cavity. The second-order correlation function of the photon emission statistics is found to be pump wavelength dependent, varying from g(2)(0) = 0.4 to 1.45, highlighting the influence of vibrational relaxation on the Jaynes-Cummings ladder. Our results show that cavity quantum electrodynamic effects can be observed in molecular systems at ambient conditions, opening significant potential for device applications.

Date: 2019
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DOI: 10.1038/s41467-019-08611-5

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