Atomically thin van der Waals crystals have recently enabled new scientific and technological breakthroughs across a variety of disciplines in materials science, nanophotonics and physics. However, non-classical photon emission from these materials has not been achieved to date. Here we report room temperature quantum emission from hexagonal boron nitride nanoflakes. The single photon emitter exhibits a combination of superb quantum optical properties at room temperature that include the highest brightness reported in the visible part of the spectrum, narrow line width, absolute photo-stability, a short excited state lifetime and a high quantum efficiency. Density functional theory modeling suggests that the emitter is the antisite nitrogen vacancy defect that is present in single and multi-layer hexagonal boron nitride. Our results constitute the unprecedented potential of van der Waals crystals for nanophotonics, optoelectronics and quantum information processing.

KeywordsHexagonal boron nitride, multilayer, single photon source, multicolor, room temperature. AbstractHexagonal boron nitride (hBN) is an emerging two dimensional material for quantum photonics owing to its large bandgap and hyperbolic properties. Here we report a broad range of multicolor room temperature single photon emissions across the visible and the near infrared spectral ranges from point defects in hBN multilayers. We show that the emitters can be categorized into two general groups, but most likely possess similar crystallographic structure. We further show two approaches for engineering of the emitters using either electron beam irradiation or annealing, and characterize their photophysical properties. The emitters exhibit narrow line widths of sub 10 nm at room temperature, and a short excited state lifetime with high brightness. Remarkably, the emitters are extremely robust and withstand aggressive annealing treatments in oxidizing and reducing environments. Our results constitute the first step towards deterministic engineering of single emitters in 2D materials and hold great promise for the use of defects in boron nitride as sources for quantum information processing and nanophotonics.

Hexagonal boron nitride (hBN) has recently emerged as a fascinating platform for room-temperature quantum photonics due to the discovery of robust visible light single-photon emitters. In order to utilize these emitters, it is necessary to have a clear understanding of their atomic structure and the associated excitation processes that give rise to this single photon emission. Here, we performed density-functional theory (DFT) and constrained DFT calculations for a range of hBN point defects in order to identify potential emission candidates. By applying a number of criteria on the electronic structure of the ground state and the atomic structure of the excited states of the considered defects, and then calculating the Huang-Rhys (HR) factor, we found that the CV defect, in which a carbon atom substitutes a boron atom and the opposite nitrogen atom is removed, is a potential emission source with a HR factor of 1.66, in good agreement with the experimental HR factor. We calculated the photoluminescence (PL) line shape for this defect and found that it reproduces a number of key features in the experimental PL lineshape.

Atomically thin van der Waals crystals have recently enabled new scientific and technological breakthroughs across a variety of disciplines in materials science, nanophotonics and physics. However, non-classical photon emission from these materials has not been achieved to date. Here we report room temperature quantum emission from hexagonal boron nitride nanoflakes. The single photon emitter exhibits a combination of superb quantum optical properties at room temperature that include the highest brightness reported in the visible part of the spectrum, narrow line width, absolute photo-stability, a short excited state lifetime and a high quantum efficiency. Density functional theory modeling suggests that the emitter is the antisite nitrogen vacancy defect that is present in single and multi-layer hexagonal boron nitride. Our results constitute the unprecedented potential of van der Waals crystals for nanophotonics, optoelectronics and quantum information processing.

Hexagonal boron nitride is a wide-band-gap van der Waals material that has recently emerged as a promising platform for quantum photonics experiments. In this work, we study the formation and localization of narrowband quantum emitters in large flakes (up to tens of micrometers wide) of hexagonal boron nitride. The emitters can be activated in as-grown hexagonal boron nitride by electron irradiation or high-temperature annealing, and the emitter formation probability can be increased by ion implantation or focused laser irradiation of the as-grown material. Interestingly, we show that the emitters are always localized at the edges of the flakes, unlike most luminescent point defects in three-dimensional materials. Our results constitute an important step on the roadmap of deploying hexagonal boron nitride in nanophotonics applications.

Quantum emitters in two-dimensional materials are promising candidates for studies of light-matter interaction and next generation, integrated on-chip quantum nanophotonics. However, the realization of integrated nanophotonic systems requires the coupling of emitters to optical cavities and resonators. In this work, we demonstrate hybrid systems in which quantum emitters in 2D hexagonal boron nitride (hBN) are deterministically coupled to high-quality plasmonic nanocavity arrays. The plasmonic nanoparticle arrays offer a high-quality, low-loss cavity in the same spectral range as the quantum emitters in hBN. The coupled emitters exhibit enhanced emission rates and reduced fluorescence lifetimes, consistent with Purcell enhancement in the weak coupling regime. Our results provide the foundation for a versatile approach for achieving scalable, integrated hybrid systems based on low-loss plasmonic nanoparticle arrays and 2D materials.

Quantum technologies require robust and photostable single photon emitters (SPEs). Hexagonal boron nitride (hBN) has recently emerged as a promising candidate to host bright and optically stable SPEs operating at room temperature. However, the emission wavelength of the fluorescent defects in hBN has, to date, been shown to be uncontrolled, with a wide spread of zero phonon line (ZPL) energies spanning a broad spectral range (hundreds of nanometers), which hinders the potential development of hBN-based devices and applications. Here we demonstrate chemical vapor deposition growth of large-area, few-layer hBN films that host large quantities of SPEs: ~100-200 per 10×10 μm 2. More than 85% of the emitters have a ZPL at (580 ± 10) nm, a distribution that is an order of magnitude narrower than reported previously. Furthermore, we demonstrate tuning of the ZPL wavelength using ionic liquid devices over a spectral range of up to 15 nm-the largest obtained to date from any solid state SPE. The fabricated devices illustrate the potential of hBN for the development of hybrid quantum nanophotonic and optoelectronic devices based on 2D materials. Solid-state, single photon emitters (SPEs) are fundamental hardware components for scalable quantum photonics with proposed applications in quantum cryptography, quantum repeater technologies and entanglement distribution. 1-5 In the past few years, major advances have been achieved in the characterization of single defects in wide-bandgap materials, 1,2,4 as well as single molecules, 6 quantum dots, 3 carbon nanotubes, 7 and more recently layered van der Waals materials. 4,8-11 However, one of the overarching challenges across all platforms is the inability to readily engineer large area (centimeter-scale) materials with uniform spatial and spectral distributions of SPEs. Such a platform is highly desirable for scalable quantum photonic architectures.

Bulk hexagonal boron nitride (hBN) is a highly nonlinear natural hyperbolic material that attracts major attention in modern nanophotonics applications. However, studies of its optical properties in the visible part of the spectrum and quantum emitters hosted by bulk hBN have not been reported to date. In this work we study the emission properties of hBN crystals in the red spectral range using sub-bandgap optical excitation. Quantum emission from defects is observed at room temperature and characterized in detail. Our results advance the use of hBN in quantum nanophotonics technologies and enhance our fundamental understanding of its optical properties.