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arXiv:2603.01107

Networking Molecular Quantum Emitters on a Single Chain : From Single to Cooperative Emitters

Jean-Baptiste Marceau, Juliette Le Balle, Christel Poujol, Frédéric Fossard, Annick Loiseau, Gaëlle Recher, Étienne Gaufrès

Published Mar 1, 2026• 0 citations
arXivHTMLPDF

Abstract

Engineering light-matter interactions between multiple free-space quantum emitters is a central challenge for scalable quantum photonic technologies. In particular, accessing regimes of coherent emitter-emitter interactions, where several emitters are coupled through a shared electromagnetic environment, is essential for coherent emission and quantum functionalities. Such interactions require precise control over emitter separation and stabilization at sub-wavelength distances, a level of spatial organization that remains extremely difficult to achieve at the molecular scale in solid-state systems. Here we introduce Encoded Quantum Chains (EQC), a one-dimensional architecture in which cooperative radiative behaviour is programmed through spatial encoding of identical molecular emitters. Organic emitters and inert spacer molecules are co-encapsulated inside dielectric boron nitride nanotubes (BNNTs), enabling statistical control of intermolecular spacing from nanometres to micrometres while enforcing dipole alignment and one-dimensional confinement. Time-resolved fluorescence under ambient conditions reveals accelerated radiative decay, enhanced emission rates per emitter, and the emergence of non-mono-exponential dynamics as spacing falls below the optical wavelength, consistent with cooperative radiative states in one dimension. Bundling of EQCs enables coupling between emitters in neighbouring BNNTs, driving a dimensional crossover toward higher-dimensional delocalisation of the excitation. This modular building-block approach provides a scalable route to engineer light-matter interactions and many-body optical phenomena in confined molecular systems, opening new opportunities for distributed single-photon sources, programmable quantum emitters, and photonic architectures for quantum technologies.

DOI
10.48550/arxiv.2603.01107

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Engineering light-matter interactions between multiple free-space quantum emitters is a central challenge for scalable quantum photonic technologies. In particular, accessing regimes of coherent emitter-emitter interactions, where several emitters are coupled through a shared electromagnetic environment, is essential for coherent emission and quantum functionalities. Such interactions require precise control over emitter separation and stabilization at sub-wavelength distances, a level of spatial organization that remains extremely difficult to achieve at the molecular scale in solid-state systems. Here we introduce Encoded Quantum Chains (EQC), a one-dimensional architecture in which cooperative radiative behaviour is programmed through spatial encoding of identical molecular emitters. Organic emitters and inert spacer molecules are co-encapsulated inside dielectric boron nitride nanotubes (BNNTs), enabling statistical control of intermolecular spacing from nanometres to micrometres while enforcing dipole alignment and one-dimensional confinement. Time-resolved fluorescence under ambient conditions reveals accelerated radiative decay, enhanced emission rates per emitter, and the emergence of non-mono-exponential dynamics as spacing falls below the optical wavelength, consistent with cooperative radiative states in one dimension. Bundling of EQCs enables coupling between emitters in neighbouring BNNTs, driving a dimensional crossover toward higher-dimensional delocalisation of the excitation. This modular building-block approach provides a scalable route to engineer light-matter interactions and many-body optical phenomena in confined molecular systems, opening new opportunities for distributed single-photon sources, programmable quantum emitters, and photonic architectures for quantum technologies.
Photon emission is the hallmark of light-matter interaction and the foundation of photonic quantum science, enabling advanced sources for quantum communication and computing. Although single-emitter radiation can be tailored by the photonic environment, the introduction of multiple emitters extends this picture. A fundamental challenge, however, is that the radiative dipole-dipole coupling rapidly decays with spatial separation, typically within a fraction of the optical wavelength. We realize distant dipole-dipole radiative coupling with pairs of solid-state optical quantum emitters embedded in a nanophotonic waveguide. We dynamically probe the collective response and identify both super- and subradiant emission as well as means to control the dynamics by proper excitation techniques. Our work constitutes a foundational step toward multiemitter applications for scalable quantum-information processing.
Quantum cooperativity is evident in light-matter platforms where quantum emitter ensembles are interfaced with confined optical modes and are coupled via the ubiquitous electromagnetic quantum vacuum. Cooperative aspects such as dipole-dipole interactions and subradiance find applications in the design of nanoscale coherent light sources and highly-reflective quantum metasurfaces made up of hundreds of optically trapped atoms, in the implementation of topological quantum optics on subwavelength arrays of emitters, in quantum metrology and quantum information. The quick bursts of radiation from a collection of quasi-indistiguishable emitters provides an alternative approach to standard lasers by introducing superradiant lasers operating at extremely low intracavity power. This tutorial provides a set of theoretical tools to tackle the behavior responsible for the onset of cooperativity in light-matter systems by extending open quantum system dynamics methods, such as the master equation and quantum Langevin equations, to electron-photon interactions in strongly coupled and correlated quantum emitters ensembles. These analytical approaches are then also extended to frequency disordered or vibronically coupled quantum emitter ensembles with wide relevance ranging from atoms in optical lattices, quantum dots in solid state environments or molecular quantum systems.
Collective light emission from many-body quantum systems is a cornerstone of quantum optics, yet its implementation in solid-state platforms operating under ambient conditions remains highly challenging. Large-bandgap van der Waals materials such as hexagonal boron nitride (hBN) host stable room-temperature single-photon emitters with narrow linewidths across a broad spectral range. However, cooperative radiative effects in this system have not been previously explored. Here we demonstrate collective emission from quantum-emitter ensembles in hBN layers when the emitters are nearly indistinguishable and positioned within a sub-wavelength proximity. Using confocal microscopy and a Hanbury Brown-Twiss (HBT) configuration, we identify both isolated emitters and ensembles activated by localized electron-beam irradiation. Time-resolved photoluminescence measurements reveal a superlinear intensity enhancement and a pronounced acceleration of the radiative decay in tightly confined ensembles, with lifetimes approaching the temporal resolution of our experimental system (about 500 ps), compared to approximately 1.85 ns for single emitters or large, spatially extended ensembles. Complementary second-order photon-correlation measurements exhibit sub-Poissonian antidip consistent with emission from a few indistinguishable emitters. The simultaneous observation of lifetime shortening and enhanced emission provides direct evidence of cooperative emission at room temperature, achieved without optical cavities or cryogenic cooling. These results establish optically active defect ensembles in hBN as a scalable solid-state platform for engineered collective quantum optics in two-dimensional materials, opening avenues toward ultrabright superradiant light sources and nonclassical photonic states for quantum technologies.
Abstract Quantum antennas couple localized quantum emitters to optical modes that can be collected, routed, and used in larger photonic systems. Their performance depends on photon delivery as well as single-photon purity, coherence, and indistinguishability. This Review connects the physics of light-matter interaction with the design of quantum-photonic interfaces. We compare semiconductor quantum dots, color centers, two-dimensional and molecular emitters, and examine plasmonic, dielectric, hybrid, cavity-coupled, and waveguideintegrated antenna architectures. We discuss how emitter position, dipole orientation, spectral matching, and material loss govern radiative enhancement and quenching, then assess performance through efficiency, brightness, photon statistics, and coupling to useful optical modes. Electromagnetic and quantum-optical modeling are considered alongside fabrication, deterministic emitter placement, and experimental characterization. We further examine how arrays and metasurfaces extend control to collective emission and quantum wavefronts, and survey applications in single-photon generation, communication, networking, computing, sensing, imaging, and ranging. Across these settings, rapid decay and strong local fields produce system-level gains only when useful photon delivery improves without compromising quantum-state quality. Low-loss design, spectral stabilization, reproducible integration, and complete photon-budget reporting emerge as priorities for scalable quantum-antenna platforms.
Single-photon sources that are bright, pure, and interference-ready are essential for quantum communication and photonic quantum information processing, but many solid-state platforms still rely on bulky optical excitation, careful alignment, and post-selection to achieve useful linewidth, stability, and brightness. Scalable quantum photonics instead requires turnkey quantum-light engines that can be triggered on demand, stabilized against environmental noise, and efficiently interfaced with fibers or photonic circuits. This review surveys recent progress in electronic and photonic integration of single quantum emitters in two-dimensional materials, focusing on localized excitonic emitters in transition metal dichalcogenides and defect-based color centers in hexagonal boron nitride. On the electronic side, we discuss electrical injection, fast modulation, electrostatic stabilization, and Stark tunability as routes to suppress blinking, spectral wandering, and charge-noise-induced broadening. On the photonic side, we review waveguide and resonator platforms that funnel emission into well-defined optical modes and, in some cases, enhance radiative rates through the Purcell effect. We connect these integration strategies to key source metrics, including single-photon purity, brightness, spectral stability, and photon indistinguishability. We conclude that the next stage of progress will depend on co-designed electronic and photonic architectures that jointly optimize on-demand operation, stabilization, tunability, and packaging-compatible optical interfacing.
Controlling light photon-by-photon is central to quantum optics. At a fundamental level, photon interactions are mediated by their coupling to atoms, and ultimate control requires deterministic light-matter interfacing of single photons to single atoms. Extending this paradigm to radiatively couple multiple individual atoms in a deterministic and scalable manner opens the arena of many-body quantum optics. Here, we realize such a setting by coherently coupling solid-state artificial atoms to a nanophotonic waveguide and demonstrate higher-order photon correlations that are controlled by the number of quantum emitters. We study the scaling of nonlinear photonic transport induced by emitter-photon scattering and demonstrate that adding a quantum emitter generates higher-order photon correlations. Specifically, we experimentally observe genuine three-photon correlations from a pair of collectively coupled emitters, while contributions from lower photon numbers are suppressed. In addition, we scale to three resonant quantum emitters coupled to the waveguide. These advancements demonstrate the onset of many-body quantum optics in waveguide quantum electrodynamics, enabling new photonic quantum simulators, the creation of many-body entangled states, and the exploration of novel quantum phase transitions.