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Nature Communications

Photonic-circuited resonance fluorescence of single molecules with an ultrastable lifetime-limited transition

Penglong Ren, Shangming Wei, Weixi Liu, Shupei Lin, Zhaohua Tian, Tai‐Lin Huang, Jianwei Tang, Yaocheng Shi, Xuewen Chen

Published Jul 9, 2022• 23 citations
Publisher

Abstract

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.

DOI
10.1038/s41467-022-31603-x

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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.
Resonantly driven quantum emitters offer a very promising route to obtain highly coherent sources of single photons required for applications in quantum information processing (QIP). Realizing this for on-chip scalable devices would be important for scientific advances and practical applications in the field of integrated quantum optics. Here we report on-chip quantum dot (QD) resonance fluorescence (RF) efficiently coupled into a single-mode waveguide, a key component of a photonic integrated circuit, with a negligible resonant laser background and show that the QD coherence is enhanced by more than a factor of 4 compared to off-resonant excitation. Single-photon behavior is confirmed under resonant excitation, and fast fluctuating charge dynamics are revealed in autocorrelation g((2)) measurements. The potential for triggered operation is verified in pulsed RF. These results pave the way to a novel class of integrated quantum-optical devices for on-chip quantum information processing with embedded resonantly driven quantum emitters.
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.
Advances in nanotechnology provide techniques for the realisation of integrated quantum-optical circuits for on-chip quantum information processing(QIP). The indistinguishable single photons, required for such devices can be generated by parametric down-conversion, or from quantum emitters such as colour centres and quantum dots(QDs). Among these, semiconductor QDs offer distinctive capabilities including on-demand operation, coherent control, frequency tuning and compatibility with semiconductor nanotechnology. Moreover, the coherence of QD photons can be significantly enhanced in resonance fluorescence(RF) approaching at its best the coherence of the excitation laser. However, the implementation of QD RF in scalable on-chip geometries remains challenging due to the need to suppress stray laser photons. Here we report on-chip QD RF coupled into a single-mode waveguide with negligible resonant laser background and show that the coherence is enhanced compared to off-resonant excitation. The results pave the way to a novel class of integrated quantum-optical devices for on-chip QIP with embedded resonantly-driven quantum emitters.
Integrated quantum light sources in photonic circuits are envisaged as the building blocks of future on-chip architectures for quantum logic operations. While semiconductor quantum dots have been proven to be the highly efficient emitters of quantum light, their interaction with the host material induces spectral decoherence, which decreases the indistinguishability of the emitted photons and limits their functionality. Here, we show that the indistinguishability of in-plane photons can be greatly enhanced by performing resonance fluorescence on a quantum dot coupled to a photonic crystal waveguide. We find that the resonant optical excitation of an exciton state induces an increase in the emitted single-photon coherence by a factor of 15. Two-photon interference experiments reveal a visibility of 0.80 ± 0.03, which is in good agreement with our theoretical model. Combined with the high in-plane light-injection efficiency of photonic crystal waveguides, our results pave the way for the use of this system for the on-chip generation and transmission of highly indistinguishable photons.
Quantum light sources are crucial for the future of quantum photonic technologies and, among them, single photons on-demand are key resources in quantum communications and information processing. Ideal quantum emitters providing indistinguishable photons in a clocked manner, negligible decoherence and spectral diffusion, and with potential for scalability are today still a major challenge. We report on photostable and indistinguishable single photon emission from dibenzoterrylene molecules isolated in anthracene nanocrystals (DBT:Ac NCs) at 3K. The visibility of two-photon interference is preserved even when they are separated more than thirty times the excited-state lifetime, or ten fluorescence cycles. One of the advantages of organic molecules is the low-cost mass production of nominally identical emitters, that also allow for on-chip integration. These aspects combined with high spectral stability and coherence make them promising for applications and future quantum technologies.
Summary form only given. Efficient quantum light sources and non-linear optical elements at the few photon level are the basic ingredients for most applications in nano and quantum technologies. On the other hand, a scalable platform for quantum information and communication typically requires reliable light matter interfaces and on-chip integration. In this work we demonstrate the potential of a novel hybrid technology which combines single organic molecules as quantum emitters and dielectric chips, consisting of ridge waveguides and grating far-field couplers [1].Here the emitters are integrated by spin-coating onto the photonic chip. We demonstrate at room temperature the emission of single photons from DBT molecules into ridge waveguides with a branching ratio up to 40%. The overall single-photon source efficiency, including emission into the guided mode, propagation losses, and emission into a quasi-gaussian mode in free space, is estimated around 16%. These results are competitive with state-of-the-art single photon emission into propagating guided modes from solid state systems [4], while offering a novel platform with unprecedented versatility. Single waveguided photons can be readily processed on-chip or efficiently extracted into a quasi-gaussian mode in free space. We also discuss options to further improve the collection efficiency and applications to quantum optics [5] and to study manybody-induced quantum correlation effects [6].