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arXiv:2105.02560 · Physical Review Letters

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

André Pscherer, Manuel Meierhofer, Daqing Wang, Hrishikesh Kelkar, Diego Martín-Cano, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar

Published Sep 24, 2021• 74 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physrevlett.127.133603

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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.
Abstract Control of light–matter coupling at the quantum level is an enabling technique for many emerging quantum technologies. This tutorial describes recent advances in achieving efficient coupling of light with a single molecule using an optical Fabry–Perot microcavity. We demonstrate that the efficient cavity-molecule coupling converts the molecule to an effective two-level system. In this regime, a single molecule can act as a nearly perfect reflecting mirror and exhibits optical nonlinearity at the ultimate level of single photons.
The recent progress in nanotechnology [1,2] and single-molecule spectroscopy [3-5] paves the way for cost-effective organic quantum optical technologies emergent with a promise to real-life devices operating at ambient conditions. In this letter, we harness πππ-conjugated segments of an organic ladder-type polymer strongly coupled to a microcavity forming correlated collective dressed states of light, so-called of exciton-polariton condensates. We explore an efficient way for all-optical ultra-fast control over the macroscopic condensate wavefunction via a single photon. Obeying Bose statistics, exciton-polaritons exhibit an extreme nonlinearity undergoing bosonic stimulation [6] which we have managed to trigger at the single-photon level. Relying on the nature of organic matter to sustain stable excitons dressed with high energy molecular vibrations we have developed a principle that allows for single-photon nonlinearity operation at ambient conditions opening the door for practical implementations like sub-picosecond switching, amplification and all-optical logic at the fundamental limit of single light quanta.
We demonstrate highly efficient switching of optical signals between two optical fibers controlled by a single atom.The key element of our experiment is a whispering-gallery-mode bottle microresonator, which is coupled to a single atom and interfaced by two tapered fiber couplers.This system reaches the strong coupling regime of cavity quantum electrodynamics, leading to a vacuum Rabi splitting in the excitation spectrum.We systematically investigate the switching efficiency of our system, i.e., the probability that the fiber-optical switch redirects the light into the desired output.We obtain a large redirection efficiency reaching a raw fidelity of more than 60% without postselection.Moreover, by measuring the second-order correlation functions of the output fields, we show that our switch exhibits a photon-number-dependent routing capability.
A single atom in a cavity is the model system of cavity quantum electrodynamics (CQED). The strong coupling regime between the atom and cavity-confined photon corresponds to the reversible exchange of energy between the two modes, and underpins a wide range of CQED phenomena with applications in quantum information science, including for example as quantum logic gates and as sources of entangled states. An important advance was achieved recently when strong coupling between excitons and cavity photons was reported for the first time for localized quantum dots (QDs) in micron-size solid state cavities. This has significance in terms of scalability and integration with other optical devices, and could lead to the emergence of "quantum optics on a chip" technology. However the results presented so far for quantum dots are in the linear regime, corresponding to coupling to the vacuum field (vacuum Rabi splitting); they are not a true QED effect and can equally well be described by classical physics as the coupling between two oscillators. In this paper, we present evidence for a purely quantum phenomenon for the QD/cavity photon system, namely the increase in splitting of the levels when the mean number of photons in the cavity is increased. This corresponds to non-linearities on the single-photon scale: the presence of a single excitation in the cavity changes the level structure, affecting the emission energies for a second photon. Such results are a first step in demonstrating the promise of quantum dots for CQED applications.
We demonstrate highly efficient switching of optical signals between two optical fibers controlled by a single atom. The key element of our experiment is a whispering-gallery-mode bottle microresonator, which is coupled to a single atom and interfaced by two tapered fiber couplers. This system reaches the strong coupling regime of cavity quantum electrodynamics, leading to a vacuum Rabi splitting in the excitation spectrum. We systematically investigate the switching efficiency of our system, i.e., the probability that the fiber-optical switch redirects the light into the desired output. We obtain a large redirection efficiency reaching a raw fidelity of more than 60% without postselection. Moreover, by measuring the second-order correlation functions of the output fields, we show that our switch exhibits a photon-number-dependent routing capability.
Efficient interaction of light and matter at the ultimate limit of single photons and single emitters is of great interest from a fundamental point of view and for emerging applications in quantum engineering. However, the difficulty of generating single-photon streams with specific wavelengths, bandwidths, and power as well as the weak interaction probability of a single photon with an optical emitter pose a formidable challenge toward this goal. Here, we demonstrate a general approach based on the creation of single photons from a single emitter and their use for performing spectroscopy on a second emitter situated at a distance. While this first proof of principle realization uses organic molecules as emitters, the scheme is readily extendable to quantum dots and color centers. Our work ushers in a new line of experiments that provide access to the coherent and nonlinear couplings of few emitters and few propagating photons.