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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.
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Hexagonal 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.
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.
Artificial atomic systems in solids are becoming increasingly important building blocks in quantum information processing and scalable quantum nanophotonic networks. Yet, synthesis of color centers that act as single photon emitters which are suitable for on-chip applications is still beyond reach. Here, we report a number of plasma and thermal annealing methods for the fabrication of emitters in tape-exfoliated hexagonal boron nitride (hBN) crystals. A two-step process comprised of Ar plasma etching and subsequent annealing in Ar is highly robust, and yields a seven-fold increase in the concentration of emitters in hBN. The initial plasma etching step generates emitters that suffer from blinking and bleaching, whereas the two-step process yields emitters that are photostable at room temperature and have an emission energy distribution that is red-shifted relative to that of pristine hBN. An analysis of emitters fabricated by a range of plasma and annealing treatments, combined with a theoretical investigation of point defects in hBN indicates that single photon emitters characterized by a high degree of photostability and emission wavelengths greater than ~700 nm are associated with defect complexes that contain oxygen. This is further confirmed by generating the emitters by annealing hBN in an oxidative atmosphere. Our findings advance present understanding of the structure of quantum emitter in hBN and enhance the nanofabrication toolkit that is needed to realize integrated quantum nanophotonics based on 2D materials.
Two-dimensional hexagonal boron nitride offers intriguing opportunities for advanced studies of light-matter interaction at the nanoscale, specifically for realizations in quantum nanophotonics. Here, we demonstrate the engineering of optically-addressable spin defects based on the negatively-charged boron vacancy center. We show that these centers can be created in exfoliated hexagonal boron nitride using a variety of focused ion beams (nitrogen, xenon and argon), with nanoscale precision. Using a combination of laser and resonant microwave excitation, we carry out optically detected magnetic resonance spectroscopy measurements, which reveal a zero-field ground state splitting for the defect of ~3.46 GHz. We also perform photoluminescence excitation spectroscopy and temperature dependent photoluminescence measurements to elucidate the photophysical properties of the center. Our results are important for advanced quantum and nanophotonics realizations involving manipulation and readout of spin defects in hexagonal boron nitride.
Single photon emitters in 2D hexagonal boron nitride (hBN) have attracted a considerable attention because of their highly intense, stable, and strain-tunable emission. However, the precise source of this emission, in particular the detailed atomistic structure of the involved crystal defect, remains unknown. In this work, we present first-principles calculations of the vibrationally resolved optical fingerprint of the spin-triplet (2)(_^3)B_1 to (1)(_^3)B_1 transition of the VNCB point defect in hBN. Based on the excellent agreement with experiments for key spectroscopic quantities such as the emission frequency and polarization, the photoluminescence (PL) line shape, Huang-Rhys factor, Debye-Waller factor, and re-organization energy, we conclusively assign the observed single photon emission at ~2eV to the VNCB defect. Our work thereby resolves a long-standing debate about the exact chemical nature of the source of single photon emission from hBN and establishes the microscopic understanding necessary for controlling and applying such photons for quantum technological applications.
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