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European Quantum Electronics Conference (EQEC)

Coherent optical dipole coupling of two individual molecules at nanometre separation

Christian Hettich, J. Zitzmann, Ilja Gerhardt, Vahid Sandoghdar, C. Schmitt

Published Jan 1, 2003• 1 citation
Publisher

Abstract

A novel approach that combines high resolution laser spectroscopy with scanning probe microscopy to determine the locations of individual fluorescent molecules in all three dimensions with nanometer accuracy and to study their optical interaction is reported. The schematic arrangement of the setup is described. Applying the technique, two individual molecules are located that are separated by 12 /spl plusmn/ 2 nm. In addition, it is shown that these two molecules are coupled via the coherent dipole-dipole coupling, leading to two sub- and superradiant states. By increasing the intensity of the incident laser beam, a two-photon transition is put into evidence that takes place at the frequency midway between the original transition frequencies of the system. Finally, photon statistics of the fluorescence light is measured and photon bunching is observed when exciting the system at the new frequency whereas excitation of the system at any of the original resonances yields photon antibunching.

DOI
10.1109/eqec.2003.1314187

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A novel approach that combines high resolution laser spectroscopy with scanning probe microscopy to determine the locations of individual fluorescent molecules in all three dimensions with nanometer accuracy and to study their optical interaction is reported. The schematic arrangement of the setup is described. Applying the technique, two individual molecules are located that are separated by 12 /spl plusmn/ 2 nm. In addition, it is shown that these two molecules are coupled via the coherent dipole-dipole coupling, leading to two sub- and superradiant states. By increasing the intensity of the incident laser beam, a two-photon transition is put into evidence that takes place at the frequency midway between the original transition frequencies of the system. Finally, photon statistics of the fluorescence light is measured and photon bunching is observed when exciting the system at the new frequency whereas excitation of the system at any of the original resonances yields photon antibunching.
By performing cryogenic laser spectroscopy under a scanning probe electrode that induces a local electric field, we have resolved two individual fluorescent molecules separated by 12 nanometers in an organic crystal. The two molecules undergo a strong coherent dipole-dipole coupling that produces entangled sub- and superradiant states. Under intense laser illumination, both molecules are excited via a two-photon transition, and the fluorescence from this doubly excited system displays photon bunching. Our experimental scheme can be used to optically resolve molecules at the nanometer scale and to manipulate the degree of entanglement among them.
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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.
Single terrylene molecules embedded in microscopic p-terphenyl crystals are identified with the technique of fluorescence excitation spectroscopy. By use of the architecture of a scanning-probe microscope at T = 1.4 K , a single molecule is scanned through an excitation laser beam while the fluorescence signal is recorded. In this manner we have mapped the intensity distribution in a one-dimensional optical standing wave, demonstrating the potential of a single molecule as a nanometric probe. We discuss future experiments aimed at combining the high spatial and spectral sensitivity of a single molecule.
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.
Using quantum emitters (such as quantum dots, atoms, NV defects in diamond ...) in order to create quantum logic gates, is a widely studied topic in modern physics. Among all of those objects, organic molecules trapped in condensed matter are nearly ideal quantum emitters dispensing single indistinguishable photons. Moreover, at low temperature (≈ 2K), molecules are very well modelized by a two-level system. At nanometric distances, two molecules can be coupled by the dipole-dipole interaction leading to the apparition of two delocalized states respectively sub- and super-radiant. The observation of two coupled dipoles has been reported only once in the literature in 2002, despite of numerous interesting applications for quantum computing. The major limitation is the low probability to find an entangled pair in a sample. For this purpose, we lately developed an optical nanoscopy method based on the saturation of the excited state by a scanned donut shaped beam, and operating at cryogenic temperature, allowing us to find some pairs of coupled dipoles. We obtained a sub 10-nm resolution for a single dipole imaging. When the donut is scanned over an entangled pair, the Rabi frequencies seen by the two emitters varies which modifies the four energy levels of the pair by AC lightshift and leads to the apparition of fluorescence dips in the final image, when two levels become degenerated. With this technique we succeeded in doing specific images of an entangled system delocalized over 20 nm. The goal of the research activity presented here is to manipulate, on demand, the degree of entanglement of such a system. The latter could only be changed by applying an external electric field on the pair, which tunes the energy difference of the two emitters by Stark effect. We have been able to put at resonance the two emitters and observed a broadening and shrinking of the symmetric and antisymmetric transitions compatible with a modification of theirs relative lifetimes.