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arXiv:2301.11024

On-chip interference of scattering from two individual molecules in plastic

Dominik Rattenbacher, Alexey Shkarin, Jan Renger, Tobias Utikal, Stephan Götzinger, Vahid Sandoghdar

Published Jan 26, 2023• 0 citations
arXivHTMLPDF

Abstract

Integrated photonic circuits offer a promising route for studying coherent cooperative effects of a controlled collection of quantum emitters. However, spectral inhomogeneities, decoherence and material incompatibilities in the solid state make this a nontrivial task. Here, we demonstrate efficient coupling of a pair of organic molecules embedded in a plastic film to a TiO$_2$ microdisc resonator on a glass chip. Moreover, we tune the resonance frequencies of the molecules with respect to that of the microresonator by employing nanofabricated electrodes. For two molecules separated by a distance of about 8$\,μ$m and an optical phase difference of about $π/2$, we report on a large collective extinction of the incident light in the forward direction and the destructive interference of its scattering in the backward direction. Our work sets the ground for the coherent coupling of several molecules via a common mode and the realization of polymer-based hybrid quantum photonic circuits.

DOI
10.48550/arxiv.2301.11024

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Integrated photonic circuits offer a promising route for studying coherent cooperative effects of a controlled collection of quantum emitters. However, spectral inhomogeneities, decoherence and material incompatibilities in the solid state make this a nontrivial task. Here, we demonstrate efficient coupling of a pair of organic molecules embedded in a plastic film to a TiO2_22​ microdisc resonator on a glass chip. Moreover, we tune the resonance frequencies of the molecules with respect to that of the microresonator by employing nanofabricated electrodes. For two molecules separated by a distance of about 8 μ\,μμm and an optical phase difference of about π/2π/2π/2, we report on a large collective extinction of the incident light in the forward direction and the destructive interference of its scattering in the backward direction. Our work sets the ground for the coherent coupling of several molecules via a common mode and the realization of polymer-based hybrid quantum photonic circuits.
Integrated photonic circuits offer a promising route for studying coherent cooperative effects of a controlled collection of quantum emitters. However, spectral inhomogeneities, decoherence, and material incompatibilities in the solid state make this a nontrivial task. Here, we demonstrate efficient coupling of a pair of Fourier-limited organic molecules embedded in a polyethylene film to a TiO2 microdisc resonator on a glass chip. Moreover, we tune the resonance frequencies of the emitters with respect to that of the microresonator by employing nanofabricated electrodes. For two molecules separated by a distance of about 8 µm and an optical phase difference of about π/2, we report on a large collective extinction of the incident light in the forward direction and the destructive interference of its scattering in the backward direction. Our work sets the ground for coherent coupling of several quantum emitters via a common mode and realization of polymer-based hybrid quantum photonic circuits.
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].
We implement permanent spectral tuning to bring lifetime-limited emitters into collective resonance within an integrated photonic cavity. This addresses a fundamental challenge in solid-state cavity QED: combining multiple coherent quantum emitters with scalable nanophotonics. Our hybrid approach decouples emitter synthesis from nanophotonic fabrication using straightforward techniques that make cavity QED broadly accessible. High doping densities allow us to couple several coherent emitters to a single cavity mode, while optically-induced frequency shifting provides long-lived spectral control. By tuning two molecules into resonance, we demonstrate controlled formation of collective quantum states, establishing a scalable platform for many-body cavity QED. This opens pathways toward chemically-designed quantum systems where optical properties are engineered through synthetic chemistry.
We present a hybrid solid-state cavity quantum electrodynamics (QED) platform that integrates a high density of coherent organic molecules with high-quality-factor nanophotonics. Thin anthracene crystals doped with dibenzoterrylene (DBT) are mechanically transferred onto prefabricated silicon nitride photonic crystal cavities, preserving both the cavity quality and molecular coherence. This approach decouples emitter synthesis from nanofabrication, providing a pathway for integrating other types of emitters. The high density of molecular emitters results in up to ten molecules being coupled to a single cavity. By tuning pairs of molecules into resonance within a single cavity mode, we observe cavity-mediated interactions in both dispersive and dissipative regimes. These results establish an accessible route to deterministic on-chip single- and multiphoton sources.
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.