Quantum electrodynamics at room temperature coupling a single vibrating molecule with a plasmonic nanocavity.
Deacon, William D
Turek, Vladimir A
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Ojambati, F., Chikkaraddy, R., Deacon, W. D., Horton, M., Kos, D., Turek, V. A., Keyser, U., & et al. (2019). Quantum electrodynamics at room temperature coupling a single vibrating molecule with a plasmonic nanocavity.. Nature communications, 10 (1), 1049. https://doi.org/10.1038/s41467-019-08611-5
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.
European Research Council (320503)
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External DOI: https://doi.org/10.1038/s41467-019-08611-5
This record's URL: https://www.repository.cam.ac.uk/handle/1810/288733