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Coherent Coupling of Single Organic Dye Molecules to Optical Nanoguides

Pierre Türschmann

Published Jan 1, 2018• 2 citations
Publisher

Abstract

Optical studies of single emitters have become routine for a number of systems ranging from atoms and ions in the gas phase to molecules, color centers and quantum dots in the solid-state. A new direction in experimental quantum optics is to exploit this know-how to assemble well-defined arrangements of optically coupled emitters for investigating quantum many-body physics. However, common approaches via strong focusing or cavity quantum electrodynamics do not scale favorably. We developed a scalable light-matter interface by coupling organic dye molecules to subwavelength dielectric waveguides (nanoguides). Their small effective mode area gives rise to substantial single-emitter coupling efficiencies with expected values up to 35%. By combining high-resolution microscopy with fluorescence excitation and resonance fluorescence spectroscopy, we study the coupled nano-guide-emitter system. Our results demonstrate the versatility of the geometry for reaching high optical densities and yet maintaining the addressability of each single emitter. We show that we can couple several thousand molecules simultaneously and coherently to a single guided mode, while their nearly lifetime-limited resonances are inhomogeneously distributed. The optical response of the coupled nanoguide-emitter system can be controlled by modifying the molecular electronic states either via static electric or external optical fields. Here, a pump beam can switch and even coherently amplify a weak laser beam that probes the inherent nonlinearity of a single molecule. Moreover, we gain local control of the molecular resonance frequencies via the dc Stark effect by applying static electric fields on microelectrodes integrated along our chip-compatible nanoguides. Exploiting this tunability allows us to match the resonance frequencies of two molecules that are coherently coupled to the same waveguide mode. All these crucial ingredients, a scalable light-matter interface, high optical densities, external control over the molecular resonance frequencies and their nonlinear response, open up realistic prospects for investigating small, but well-defined networks of quantum emitters coherently coupled via a shared guided mode.

DOI
10.25593/978-3-96147-097-6

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Optical studies of single emitters have become routine for a number of systems ranging from atoms and ions in the gas phase to molecules, color centers and quantum dots in the solid-state. A new direction in experimental quantum optics is to exploit this know-how to assemble well-defined arrangements of optically coupled emitters for investigating quantum many-body physics. However, common approaches via strong focusing or cavity quantum electrodynamics do not scale favorably. We developed a scalable light-matter interface by coupling organic dye molecules to subwavelength dielectric waveguides (nanoguides). Their small effective mode area gives rise to substantial single-emitter coupling efficiencies with expected values up to 35%. By combining high-resolution microscopy with fluorescence excitation and resonance fluorescence spectroscopy, we study the coupled nano-guide-emitter system. Our results demonstrate the versatility of the geometry for reaching high optical densities and yet maintaining the addressability of each single emitter. We show that we can couple several thousand molecules simultaneously and coherently to a single guided mode, while their nearly lifetime-limited resonances are inhomogeneously distributed. The optical response of the coupled nanoguide-emitter system can be controlled by modifying the molecular electronic states either via static electric or external optical fields. Here, a pump beam can switch and even coherently amplify a weak laser beam that probes the inherent nonlinearity of a single molecule. Moreover, we gain local control of the molecular resonance frequencies via the dc Stark effect by applying static electric fields on microelectrodes integrated along our chip-compatible nanoguides. Exploiting this tunability allows us to match the resonance frequencies of two molecules that are coherently coupled to the same waveguide mode. All these crucial ingredients, a scalable light-matter interface, high optical densities, external control over the molecular resonance frequencies and their nonlinear response, open up realistic prospects for investigating small, but well-defined networks of quantum emitters coherently coupled via a shared guided mode.
Summary form only given. A current challenge and trend in optical sciences is to extend the toolbox generated from experiments with single emitters and single photons towards interfacing photons with a well-defined number of quantum emitters. The resulting complex optical network would enable studies of many-body quantum optical phenomena and could lend itself to quantum simulations. However, common light-matter interfaces via strong focusing or cavity enhancement do not scale favourably. Therefore, achieving many-body coupling while preserving control of the individual quantum systems poses remarkable experimental challenges.Here, we present an inherently scalable platform, which relies on the evanescent coupling of single dye molecules to subwavelength TiO2waveguides (nanoguides) that are embedded in an organic matrix (Fig. 1a). At liquid helium temperatures, we observe lifetime-limited linewidths for these molecules distributed over an inhomogeneously broadened spectrum. However, by using integrated microelectrodes, we can Stark shift the resonances over a large bandwidth. The dopant concentration determines the optical density of our system which can reach up to a few hundred molecules per cubic wavelength. The highly confined mode of a nanoguide allows a substantial mode overlap with the emission pattern of a single emitter, resulting in coupling efficiencies of up to 32%. Therefore, we can observe coherent extinction signals from many different molecules in the transmission signal of a nanoguide; an example is shown by the blue curve in Fig. 1b [1]. The green and red curves in Fig. 1b demonstrate the nonlinear behaviour of a molecule when driven with a second narrow-band laser [1, 2]. We show that by modifying the spectral properties of the molecules either via external optical or static electric fields we control the optical response of a nanoguide. In addition to discussing subtleties of design and fabrication, we elaborate on future efforts towards the realization of on-chip polaritonic states [3] and the integration of further optical elements such as micoresonators [4].
Many of the currently pursued experiments in quantum optics would greatly benefit from a strong interaction between light and matter. Here, we present a simple new scheme for the efficient coupling of single molecules and photons. A glass capillary with a diameter of 600 nm filled with an organic crystal tightly guides the excitation light and provides a maximum spontaneous emission coupling factor (β) of 18% for the dye molecules doped in the organic crystal. A combination of extinction, fluorescence excitation, and resonance fluorescence spectroscopy with microscopy provides high-resolution spatiospectral access to a very large number of single molecules in a linear geometry. We discuss strategies for exploring a range of quantum-optical phenomena, including polaritonic interactions in a mesoscopic ensemble of molecules mediated by a single mode of propagating photons.
The authors developed a new solid-state platform for nanoguide-QED in which both high optical densities and single emitter addressability are achieved. The work has succeeded in embedding organic dye molecules inside the tight mode of a dielectric nanoguide. The results pave the way for the integration of organic quantum emitters into more complex nanocircuits, which enables the combination of single molecule spectroscopy with other quantum optical systems and the realization of hybrid quantum networks.
Resonance fluorescence as the emission of a resonantly-excited two-level quantum system promises indistinguishable single photons and coherent high-fidelity quantum-state manipulation of the matter qubit, which underpin many quantum information processing protocols. Real applications of the protocols demand high degrees of scalability and stability of the experimental platform, and thus favor quantum systems integrated on one chip. However, the on-chip solution confronts several formidable challenges compromising the scalability prospect, such as the randomness, spectral wandering and scattering background of the integrated quantum systems near heterogeneous and nanofabricated material interfaces. Here we report an organic-inorganic hybrid integrated quantum photonic platform that circuits background-free resonance fluorescence of single molecules with an ultrastable lifetime-limited transition. Our platform allows a collective alignment of the dipole orientations of many isolated molecules with the photonic waveguide. We demonstrate on-chip generation, beam splitting and routing of resonance-fluorescence single photons with a signal-to-background ratio over 3000 in the waveguide at the weak excitation limit. Crucially, we show the photonic-circuited single molecules possess a lifetime-limited-linewidth transition and exhibit inhomogeneous spectral broadenings of only about 5% over hours' measurements. These findings and the versatility of our platform pave the way for scalable quantum photonic networks.
At the quantum limit of nonlinear optics, where single photons interact with individual emitters, new phenomena are found. One-dimensional, subwavelength waveguides have recently emerged as a promising quantum optical platform capable of both guiding and confining photons, leading to efficient light-matter interactions and enhancing quantum optical nonlinearities. We explore this regime using both single organic molecules and epitaxially grown quantum dots coupled to nanoscale waveguides. In the first case, two-color experiments allow us to observe distinctly quantum nonlinearities such as Stark shifts of the molecular resonances or amplification without population inversion, although we are limited by relatively weak molecule-waveguide coupling. In contrast, quantum dots can be nearly perfectly coupled to waveguides, allowing us to demonstrate optical nonlinearities at the true single photon level. These, as we discuss, can be used as a basis for novel on-chip quantum technologies.
Many interesting proposals in quantum optics and light-matter interaction rely on having multiple quantum emitters well-coupled to a single mode of light. Of particular interest are cases where several identical emitters couple to a one-dimensional (1D) photonic medium. Recently, we presented such a system by evanescent coupling of organic dye molecules to the same guided mode of an on-chip subwavelength waveguide [1]. While this coupling allowed us to demonstrate up to 7.5% transmission extinction of the propagating light by a single molecule, it is still not sufficient for achieving higher-order effects such as photon-mediated interaction of multiple emitters coupled to the same waveguide.