strong coupling

semiconductor microcavities

quantum emitters

stimulated raman

four-wave mixing

optical bistability

optical switch

second harmonic

induced transparency

Physical Review Letters

A single quantum emitter can possess a very strong intrinsic nonlinearity, but its overall promise for nonlinear effects is hampered by the challenge of efficient coupling to incident photons. Common nonlinear optical materials, on the other hand, are easy to couple to but are bulky, imposing a severe limitation on the miniaturization of photonic systems. In this Letter, we show that a single organic molecule acts as an extremely efficient nonlinear optical element in the strong coupling regime of cavity quantum electrodynamics. We report on single-photon sensitivity in nonlinear signal generation and all-optical switching. Our work promotes the use of molecules for applications such as integrated photonic circuits operating at very low powers.Received 4 May 2021Accepted 12 August 2021DOI:https://doi.org/10.1103/PhysRevLett.127.133603Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Open access publication funded by the Max Planck Society.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasLight-matter interactionNonlinear opticsQuantum opticsAtomic, Molecular & Optical

Single-Molecule Vacuum Rabi Splitting: Four-Wave Mixing and Optical Switching at the Single-Photon Level