Cavity QED with molecular defects coupled to a photonic crystal cavity
Christian Lange, Arya Deepak Keni, Ishita Agarwal, Emma Daggett, Adhyyan S. Mansukhani, Kundu, Ankit, Benjamin W. Cerjan, Libai Huang, Jonathan D. Hood
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 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.
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.
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].
Efficient interfaces between optical photons and quantum bits are fundamental building blocks for quantum networks and large-scale quantum computers. We demonstrate an integrated platform for scalable quantum optics based on color centers coupled to diamond nanodevices. First, we incorporate nitrogen-vacancy (NV) centers in diamond into hybrid nanophotonic crystal cavities. Despite our progress towards coupling the NV to cavity photons, we find that the NV-cavity interface is limited by the imperfections of the color center's properties and its local environment. We approach this challenge first by characterizing and modifying the diamond surface to reduce the environmental noise affecting the NV optical transition. Subsequently, we develop a new approach that makes use of a quantum emitter with intrinsic protection from this noise: the silicon-vacancy (SiV) center in diamond. We demonstrate that SiV centers introduced through ion implantation feature highly coherent optical transitions, even inside nanostructures. By placing SiV centers inside all-diamond photonic crystal cavities, we achieve strong SiV-photon coupling with a cooperativity of greater than 20. Using this platform, we realize a quantum-optical switch controlled by the spin degree of freedom of a single SiV. By measuring intensity correlations of indistinguishable Raman photons emitted into a single waveguide, we observe a quantum interference effect resulting from the superradiant emission of two probabilistically entangled SiV centers. Finally, we demonstrate controllable photon-mediated interactions between the spin degrees of freedom of two cavity-coupled SiV centers. When the optical transitions of the two SiV centers are tuned into resonance, the coupling of each SiV to the common cavity mode results in a coherent interaction between the two SiVs, leading to the observation of super- and sub-radiant two-SiV states.
ABSTRACT Integrated quantum photonics is rapidly emerging as a transformative platform for realizing scalable, chip‐based quantum technologies, from secure communication to advanced sensing and computing. At the heart of this revolution are solid‐state quantum emitters: atom‐like light sources embedded in a variety of host materials that enable single‐photon generation, quantum interference, and spin–photon coupling. We begin by discussing quantum emitters across bulk crystals, van der Waals materials, and chemically synthesized nanostructures, highlighting their performance trade‐offs and integration potential. We then examine nanophotonic cavities that enhance the light‐matter interaction, from photonic crystals to metasurfaces and Moiré resonators. Next, we discuss fabrication techniques with sub‐10 nm precision, including material‐specific etching strategies and hybrid integration schemes. Finally, we address emerging approaches for deterministic placement, cavity tuning, and on‐chip scalability. By bringing together insights from materials science, nanofabrication, and quantum optics, this Review provides a comprehensive perspective on the design and integration of high‐performance quantum emitters for scalable photonic platforms.
Color centers are optically active point defects in semiconductor materials, many of them carrying a spin degree of freedom that couples coherently to emitted photons. This makes them a leading candidate for building quantum computers, networks, and sensors, but realizing that promise depends on the interface between the emitter and light. Color centers must be integrated into nanophotonic structures, such as nanopillars that collect their emission efficiently and optical cavities that couple them to a single mode. This dissertation studies the physics of quantum emitters inside such structures along two complementary threads: the direct cryogenic spectroscopy of color centers integrated into silicon carbide nanostructures, and the study of the physics of many-body cavity quantum electrodynamics (CQED) through simulation on superconducting and trapped-ion quantum hardware. The first thread concerns the nitrogen-vacancy (NV) center in 4H silicon carbide integrated into nanopillars. We show that the sub-wavelength geometry of a nanopillar reshapes the local electromagnetic environment, granting optical access to transitions that selection rules forbid in bulk material: emission from the PL3 divacancy, nearly absent in planar devices, becomes pronounced in nanopillars through a polarization transformation of the excitation field, and the orientation-dependent collection of the pillar resolves the previously ambiguous NV4′ line, establishing nanophotonic integration as a symmetry-sensitive probe of defect structure. We then take up the complementary problem of quantifying how many emitters a device contains, adapting the number-and-brightness technique from fluorescence microscopy to solid-state emitters. This calibration-free method counts dense NV ensembles in silicon carbide nanopillars, a regime beyond the reach of existing optical techniques, and extracts their areal density and formation yield. The second thread turns to many-body cavity QED, in which placing N emitters in a common cavity enhances the light-matter coupling by √N and gives rise to collective effects that are central to strong-coupling applications yet difficult to achieve in solid-state devices based on defects. We realize one such effect on a superconducting circuit, demonstrating photon blockade, the conversion of a coherent drive into a stream of single photons, in a Tavis–Cummings system of N = 1, 2, 3 transmon qubits coupled to a common resonator. To study the open-system dynamics that govern these systems, we digitally simulate the dissipative Tavis–Cummings model on both a superconducting and a trapped-ion processor. Platform-specific compilation and error mitigation yield population dynamics in close agreement with exact solutions, providing a recipe for simulating cavity-emitter systems on contemporary quantum computers. Together, the two threads connect the fabrication and characterization of color-center devices to the many-body cavity-QED physics that will ultimately govern their performance.