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.
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.
Engineering the photonic environment using lattices of coupled resonators, which we refer to as lattice quantum electrodynamics (QED), provides a route to control both the spontaneous emission of individual quantum emitters and the photon-mediated interactions between them. Here we introduce an optical lattice QED platform based on individual dibenzoterrylene (DBT) molecules embedded in anthracene crystals and coupled to lattices of open optical microcavities. This hybrid architecture benefits from narrow-linewidth molecular emitters, site-resolved optical access, engineered coupled-resonator bands, and compatibility with established molecular frequency-tuning techniques. As a proof-of-principle demonstration, we observe emitter-photon bound states formed when the optical transition of a single molecule is tuned to the band gap of a Su-Schrieffer-Heeger (SSH) cavity lattice. These in-gap states display directional localization and photon emission on a single sublattice, inherited from the vacancy-induced topological edge modes of the underlying SSH lattice. Our results establish open-cavity lattices coupled to DBT molecules as a versatile architecture for engineering many-emitter quantum optical systems with controllable photon-mediated interactions.
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.
Quantum light-matter interactions form the basis of many quantum technologies and much fundamental research. Organic molecules are an impressive platform for the generation of quantum light, both as single photon emitters and as collective systems. In this work, I investigate quantum light-matter interactions with molecules of dibenzoterrylene in crystals of anthracene. I outline methods to grow dibenzoterrylene-doped anthracene crystals, and I characterize the optical properties of cryogenically cooled molecules. I prepare collective systems composed of pairs of molecules interacting through their free-space electromagnetic fields. I demonstrate a method to tune interacting molecules into resonance to form superradiant and subradiant collective states. Finally, I present a platform for solid-state cavity QED based on molecules of dibenzoterrylene coupled to a nanophotonic cavity. This demonstration establishes a route toward scalable deterministic photon generation with molecules. I also tune pairs of cavity-coupled molecules into resonance to form distributed collective states, opening the door to cavity-mediated many-body interactions.
The on-chip integration of quantum light sources and nonlinear elements constitutes a major step toward scalable photon-based quantum information processing and communication. In this work we demonstrate the potential of a hybrid technology that combines organic-molecule-based quantum emitters and dielectric chips consisting of ridge waveguides and grating far-field couplers. In particular, dibenzoterrylene molecules in thin anthracene crystals are used as single-photon sources, exhibiting long-term photostability, easy fabrication methods, almost unitary quantum yield, and lifetime-limited emission at cryogenic temperatures. We couple such single emitters to silicon nitride ridge waveguides, showing a coupling efficiency of up to 42 ± 2% over both propagation directions. Our results open a novel path toward a fully integrated and scalable photon-processing platform.
Organic molecules embedded in an organic matrix exhibit lifetime-limited optical coherence and bright emission at cryogenic temperatures below 3 K. Here we present a simple vapor-phase growth method for synthesizing optically thin DBT-doped anthracene crystals that are compatible with integrated nanophotonics. The crystals are ~200 nm thick with sub-nm surface roughness and a tunable lateral dimension of up to 200 μm. The molecular transitions remain narrow and spectrally stable, with inhomogeneous broadening below 100 GHz, comparable to DBT in bulk anthracene. The dopant density is tunable up to several hundred molecules per μm2, ensuring emitters within the near-field of nanophotonic structures. We demonstrate that the crystals can be micropositioned onto integrated photonic devices with the molecular dipole aligned to the optical mode. This approach opens a path toward on-chip single-photon sources and collective many-emitter effects.
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 ICT 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 [1]. Dibenzoterrylene molecules in anthracene crystals (DBT:Ac) are particularly suitable quantum systems for this task, since they exhibit long-term photostability in thin samples [2], easy fabrication methods and life-time limited emission at cryogenic temperatures [3]. 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. References [1] P. Lombardi et al., Arxiv: 1701.00459v1 (2017). [2] C. Toninelli et al., Opt. Express 18, 6577 (2010). [3] A. A. L. Nicolet et al., ChemPhysChem 8, 1929 (2007). [4] I. Zadeh et al., Nano Lett. 16, 2289 (2016); R. S. Daveau et al., Arxiv: 1610.08670v1 (2016). [5] J. Hwang et. al., New J. Phys. 13, 085009 (2011); H.-W. Lee et al., Phys. Rev. A 63, 012305 (2000).