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arXiv:1909.02648

Coupling of deterministically activated quantum emitters in hexagonal boron nitride to plasmonic surface lattice resonances

Nicholas V. Proscia, Collison, Robert J., Carlos A. Meriles, Vinod M. Menon

Published Sep 5, 2019• 242 citations
arXivHTMLPDF

Abstract

Cooperative phenomena stemming from radiation-field-mediated coupling between individual quantum emitters are presently attracting broad interest for on-chip photonic quantum memories and long-range entanglement. Common to these applications is the generation of electromagnetic modes over macroscopic distances. Much research, however, is still needed before such systems can be deployed in the form of practical devices, starting with the investigation of alternate physical platforms. Quantum emitters in two-dimensional (2D) systems provide an intriguing route because these materials can be adapted to arbitrarily shaped substrates to form hybrid systems where emitters are near-field-coupled to suitable optical modes. Here, we report a scalable coupling method allowing color center ensembles in a van der Waals material - hexagonal boron nitride - to couple to a delocalized high quality plasmonic surface lattice resonance. This type of architecture is promising for photonic applications, especially given the ability of the hexagonal boron nitride emitters to operate as single-photon sources at room temperature.

DOI
10.1515/nanoph-2019-0136

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Cooperative phenomena stemming from radiation-field-mediated coupling between individual quantum emitters are presently attracting broad interest for on-chip photonic quantum memories and long-range entanglement. Common to these applications is the generation of electromagnetic modes over macroscopic distances. Much research, however, is still needed before such systems can be deployed in the form of practical devices, starting with the investigation of alternate physical platforms. Quantum emitters in two-dimensional (2D) systems provide an intriguing route because these materials can be adapted to arbitrarily shaped substrates to form hybrid systems where emitters are near-field-coupled to suitable optical modes. Here, we report a scalable coupling method allowing color center ensembles in a van der Waals material - hexagonal boron nitride - to couple to a delocalized high quality plasmonic surface lattice resonance. This type of architecture is promising for photonic applications, especially given the ability of the hexagonal boron nitride emitters to operate as single-photon sources at room temperature.
The cooperative phenomena stemming from the radiation field-mediated coupling between individual quantum emitters are presently attracting broad interest for applications related to on-chip photonic quantum memories and long-range entanglement. Common to these applications is the generation of electro-magnetic modes over macroscopic distances. Much research, however, is still needed before such systems can be deployed in the form of practical devices, starting with the investigation of alternate physical platforms. Quantum emitters in two-dimensional (2D) systems provide an intriguing route because these materials can be adapted to arbitrarily shaped substrates to form hybrid systems wherein emitters are near-field-coupled to suitable optical modes. Here, we report a scalable coupling method allowing color center ensembles in a van der Waals material (hexagonal boron nitride) to couple to a delocalized high-quality plasmonic surface lattice resonance. This type of architecture is promising for photonic applications, especially given the ability of the hexagonal boron nitride emitters to operate as single-photon sources at room temperature.
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.
Single-photon sources are crucial components for building quantum networks and communications, but their optical coherent control remains a significant challenge in the development of quantum technologies. Recently, single-photon sources in atomically thin 2D materials such as transition metal dichalcogenides and van der Waals materials have emerged as promising solid-state quantum light emitters [1]. Hexagonal boron nitride (hBN) is a 2D insulator, which hosts optically active states in its band gap that efficiently emit single photons even at room temperature. The wide range of emission wavelengths, narrow emission lines, and convenient tunability of these hBN emitters make them particularly interesting for quantum sensing and wavelength division multiplexed quantum communications. They can also be found in commercially available nanocrystals, making them ideal for creating large arrays of single-photon emitters [2] and efficient coupling to photonic structures, such as 3D-printed microlenses [3].
Sources of pure and indistinguishable single-photons are critical for near-future optical quantum technologies. Recently, color centers hosted by two-dimensional hexagonal boron nitride (hBN) have emerged as a promising platform for high luminosity room temperature single-photon sources. Despite the brightness of the emitters, the spectrum is rather broad and the single-photon purity is not sufficient for practical quantum information processing. Here, we report integration of such a quantum emitter hosted by hBN into a tunable optical microcavity. A small mode volume of the order of λ 3 allows us to Purcell enhance the fluorescence, with the observed excited state lifetime shortening. The cavity significantly narrows the spectrum and improves the single-photon purity by suppression of off-resonant noise. The complete device, including all optics, driving electronics, and control units, is compact and integrated in a small volume of 10 × 10 × 10 cm 3, allowing for portable usage in mobile applications.
Quantum emitters in hexagonal boron nitride (hBN) are promising building blocks for solid-state quantum photonics because of their bright room-temperature emission. These emitters strongly interact with lattice vibrations, which partially underpins their excitation efficiency. Here, using complementary cathodoluminescence (CL) and photoluminescence (PL) spectroscopy, we demonstrate cavity-mediated interactions between hBN quantum emitters coupled to the same plasmonic Au void cavity at the room temperature. Cathodoluminescence measurements reveal that a vibronic transition of the 443 nm emitter hybridizes with the cavity mode, giving rise to a spectrally resolved splitting, while the neighboring 537 nm emitter remains in the weak-coupling regime despite spectral overlap. The energy split of the CL peak is at the order of 36.2 meV, whereas the PL-resolved peak is approximately 24.1 meV, which is due to the collective excitations of multiple emitters per electron excitation and their mutual interactions. Maxwell-Bloch simulations reproduce the experimental spectra and identify the observed splitting as the result of cavity-induced hybridization. Excitation-dependent PL further shows that the hybridized state can be accessed through phonon-assisted excitations below the zero-phonon transition. These results demonstrate that vibronic transitions provide an effective pathway for controlling interactions between multiple quantum emitters in hybrid plasmonic nanophotonic systems.
Color centers hosted in hexagonal boron nitride have emerged as a highly promising platform for single-photon emission and spin-photon technologies relevant to quantum communication and quantum networking. As a wide-bandgap van der Waals material, hBN can host optically active quantum defects across a broad spectral range. Here, we demonstrate a simple and scalable oxygen-plasma process that reproducibly creates single quantum emitters in hBN with blinking-free zero-phonon lines spanning the near-infrared from 700 up to 971 nm. These emitters combine MHz-level brightness, single-photon purity up to 99.9\%, and ultranarrow cryogenic linewidths down to 2.7~GHz under quasi-resonant excitation, placing them in a particularly attractive regime for quantum photonics. Photostability measurements further reveal resistance to photobleaching, sub-nm spectral stability over long timescales, and near-shot-noise-limited intensity fluctuations. Analysis of the phonon sidebands shows weak vibronic coupling and ZPL-dominated emission, with Debye--Waller factors approaching 50\%. Control experiments together with EDS elemental mapping support oxygen incorporation as a necessary ingredient in activating the NIR emitter population, while first-principles calculations identify ON_NN​VN_NN​ and ON_NN​VN_NN​H as the leading defect candidates. These results establish a high-performance NIR quantum-emitter platform in hBN for free-space quantum networking and future integrated quantum-photonic architectures.