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Register a new userIdentifying Carbon as the Source of Visible Single Photon Emission from Hexagonal Boron Nitride
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Single photon emitters (SPEs) in hexagonal boron nitride (hBN) have garnered significant attention over the last few years due to their superior optical properties. However, despite the vast range of experimental results and theoretical calculations, the defect structure responsible for the observed emission has remained elusive. Here, by controlling the incorporation of impurities into hBN and by comparing various synthesis methods, we provide direct evidence that the visible SPEs are carbon related. Room temperature optically detected magnetic resonance (ODMR) is demonstrated on ensembles of these defects. We also perform ion implantation experiments and confirm that only carbon implantation creates SPEs in the visible spectral range. Computational analysis of hundreds of potential carbon-based defect transitions suggest that the emission results from the negatively charged VBCN- defect, which experiences long-range out-of-plane deformations and is environmentally sensitive. Our results resolve a long-standing debate about the origin of single emitters at the visible range in hBN and will be key to deterministic engineering of these defects for quantum photonic devices.
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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.
Development of scalable quantum photonic technologies requires on-chip integration of components such as photonic crystal cavities and waveguides with nonclassical light sources. Recently, hexagonal boron nitride (hBN) has emerged as a promising platform for nanophotonics, following reports of hyperbolic phonon-polaritons and optically stable, ultra-bright quantum emitters. However, exploitation of hBN in scalable, on-chip nanophotonic circuits, quantum information processing and cavity quantum electrodynamics (QED) experiments requires robust techniques for the fabrication of monolithic optical resonators. In this letter, we design and engineer high quality photonic crystal cavities from hBN. We employ two approaches based on a focused ion beam method and a minimally-invasive electron beam induced etching (EBIE) technique to fabricate suspended two dimensional (2D) and one dimensional (1D) cavities with quality (Q) factors in excess of 2,000. Subsequently, we show deterministic, iterative tuning of individual cavities by direct-write, single-step EBIE without significant degradation of the Q-factor. The demonstration of tunable, high Q cavities made from hBN is an unprecedented advance in nanophotonics based on van der Waals materials. Our results and hBN processing methods open up promising new avenues for solid-state systems with applications in integrated quantum photonics, polaritonics and cavity QED experiments.
Growing interest in devices based on layered van der Waals (vdW) materials is motivating the development of new nanofabrication methods. Hexagonal boron nitride (hBN) is one of the most promising materials for studies of quantum photonics and polaritonics. Here, we report in detail on a promising nanofabrication processes used to fabricate several hBN photonic devices using a hybrid electron beam induced etching (EBIE) and reactive ion etching (RIE) technique. We highlight the shortcomings and benefits of RIE and EBIE and demonstrate the utility of the hybrid approach for the fabrication of suspended and supported device structures with nanoscale features and highly vertical sidewalls. Functionality of the fabricated devices is proven by measurements of high quality cavity optical modes (Q~1500). Our nanofabrication approach constitutes an advance towards an integrated, monolithic quantum photonics platform based on hBN and other layered vdW materials.
Luminescent defect-centers in hexagonal boron nitride (hBN) have emerged as a promising 2D-source of single photon emitters (SPEs) due to their high brightness and robust operation at room temperature. The ability to create such emitters with well-defined optical properties is a cornerstone towards their integration into on-chip photonic architectures. Here, we report an effective approach to fabricate hBN single photon emitters (SPEs) with desired emission properties in two isolated spectral regions via the manipulation of boron diffusion through copper during atmospheric pressure chemical vapor deposition (APCVD)--a process we term gettering. Using the gettering technique we deterministically place the resulting zero-phonon line (ZPL) between the regions 550-600 nm or from 600-650 nm, paving the way for hBN SPEs with tailored emission properties across a broad spectral range. Our ability to control defect formation during hBN growth provides a simple and cost-effective means to improve the crystallinity of CVD hBN films, and lower defect density making it applicable to hBN growth for a wide range of applications. Our results are important to understand defect formation of quantum emitters in hBN and deploy them for scalable photonic technologies.
Solid-state single-photon emitters (SPEs) such as the bright, stable, room-temperature defects within hexagonal boron nitride (hBN) are of increasing interest for quantum information science applications. To date, the atomic and electronic origins of
SPEs within hBN are not well understood, and no studies have reported photochromism or explored cross-correlations between hBN SPEs. Here, we combine irradiation-time dependent measures of quantum efficiency and microphotoluminescence (${mu}$PL) spectroscopy with two-color Hanbury Brown-Twiss interferometry to enable an investigation of the electronic structure of hBN defects. We identify photochromism in a hBN SPE that exhibits cross-correlations and correlated quantum efficiencies between the emission of its two zero-phonon lines.
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