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, Jeremy J. Baumberg

Research output: Contribution to journalArticlepeer-review

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.
Original languageEnglish
Article number1049
JournalNature Communications
Volume10
DOIs
Publication statusPublished - 5 Mar 2019

Fingerprint

Dive into the research topics of 'Quantum electrodynamics at room temperature coupling a single vibrating molecule with a plasmonic nanocavity'. Together they form a unique fingerprint.

Cite this