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arXiv:1001.5449 · Applied Physics Letters

Conversion of neutral nitrogen-vacancy centers to negatively charged nitrogen-vacancy centers through selective oxidation

Kai‐Mei C. Fu, Charles Santori, Paul E. Barclay, Raymond G. Beausoleil

Published Mar 22, 2010• 253 citations
arXivHTMLPDF

Abstract

The conversion of neutral nitrogen-vacancy centers to negatively charged nitrogen-vacancy centers is demonstrated for centers created by ion implantation and annealing in high-purity diamond. Conversion occurs with surface exposure to an oxygen atmosphere at 465 °C. The spectral properties of the charge-converted centers are investigated. Charge state control of nitrogen-vacancy centers close to the diamond surface is an important step toward the integration of these centers into devices for quantum information and magnetic sensing applications.

DOI
10.1063/1.3364135

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The conversion of neutral nitrogen-vacancy centers to negatively charged nitrogen-vacancy centers is demonstrated for centers created by ion implantation and annealing in high-purity diamond. Conversion occurs with surface exposure to an oxygen atmosphere at 465 °C. The spectral properties of the charge-converted centers are investigated. Charge state control of nitrogen-vacancy centers close to the diamond surface is an important step toward the integration of these centers into devices for quantum information and magnetic sensing applications.
The negatively-charged nitrogen-vacancy (NV) center is the most studied optical center in diamond and is very important for applications in quantum information science. Many proposals for integrating NV centers in quantum and sensing applications rely on their tailored fabrication in ultra pure host material. In this study, we use ion implantation to controllably introduce nitrogen into high purity, low nitrogen chemical vapor deposition diamond samples. The properties of the resulting NV centers are studied as a function of implantation temperature, annealing temperature, and implantation fluence. We compare the implanted NV centers with native NV centers present deep in the bulk of the as-grown samples. The results for implanted NV centers are promising but indicate, at this stage, that the deep native NV centers possess overall superior optical properties. In particular, the implanted NV centers obtained after annealing at 2000 °C under a stabilizing pressure of 8 GPa showed an ensemble linewidth of 0.17 nm compared to 0.61 nm after annealing at 1000 °C. Over the same temperature range, the ensemble NV−/NV0 ratio increased by a factor of ∼5, although this was accompanied by an overall decrease in the NV count.
Abstract We investigated the charge state stability and coherence properties of near-surface single nitrogen vacancy (NV) centers in 12 C-enriched diamond for potential use in nanoscale magnetic field sensing applications. The stability of charge states in negatively charged NV centers (NV − ) was evaluated using one of the pulsed optically detected magnetic resonance measurements, Rabi oscillation measurements. During the accumulation of Rabi oscillations, an unstable shallow NV − was converted to a neutral state. As a result, the contrast of Rabi oscillations degraded, depending on charge state stability. We stabilized the NV − state of very shallow NV centers (∼2.6 ± 1.1 nm from the surface) created by 1.2 keV nitrogen ion implantation by diamond surface modification, UV/ozone exposure, and oxygen annealing. This improvement indicates that we can suppress the upward surface band bending and surface potential fluctuations through Fermi level pinning originating from oxygen-terminated diamond surfaces.
Etching experiments were performed that reveal the vertical distribution of optically active nitrogen-vacancy (NV) centers in diamond created in close proximity to a surface through ion implantation and annealing. The NV distribution depends strongly on the native nitrogen concentration, and spectral measurements of the neutral and negatively charged NV peaks give evidence for electron depletion effects in lower-nitrogen material. The results are important for potential quantum information and magnetometer devices where NV centers must be created in close proximity to a surface for coupling to optical structures.
Precise control over the spatial distribution and charge state of nitrogen-vacancy (NV) centers in diamond is a key requirement for further advancing this platform in quantum sensing and photonic applications. Here, we investigate nitrogen ion implantation as a scalable method to engineer NV centers in bulk single-crystalline (SC) and a 5 μ m -thick polycrystalline (PC) diamond membrane. Nitrogen-doped regions (1–80 ppm) were fabricated using a 0.7 MeV ion beam and high-temperature annealing, with NV center formation verified by confocal fluorescence imaging and spectral analysis. In SC bulk diamond, we estimate the NV concentration from spectral analysis and model the fluorescence response as a function of implantation dose, capturing both the initial increase at low concentrations and a saturation behavior at higher doses due to quenching mechanisms. In contrast, PC diamond membranes show a weaker dependence at low implantation fluences, consistent with pre-existing nitrogen impurities, thus making a statistical model significantly more complex. The activation yield is found to be of order of 1%, which is lower than in N-rich diamond samples, as implanted N is predominantly interstitial. Photoluminescence spectroscopy indicates that NV 0 is the dominant charge state in both materials, with a laser-power-dependent redistribution between neutral and negative charge states. Optically detected magnetic resonance (ODMR) measurements in SC bulk diamond resolve the hyperfine structure and allow extraction of the dephasing time ( T 2 ∗ ), while in PC diamond membranes, where NV centers tend do form near the grain boundaries, the ODMR signals are observed but spectral resolution is currently limited by impurities, grain-dependent NV orientations, and photoluminescence background.
Quantum information applications place stringent demands on the development of platforms that can host them. Color centers in diamond have been identified as important media for quantum information processing. Accordingly, the photoluminescence properties of nitrogen-vacancy (N-V) centers in diamond created by implantation and annealing are studied at cryogenic temperatures (below 10 K). We examine high pressure high temperature and chemical vapor deposition synthetic diamonds with varying nitrogen concentration and present an accurate method to estimate the concentration of the (N-V) centers created by ion implantation. The ion irradiation route produced up to 6 ppm of optically active (N-V) centers, while nitrogen implantation yielded up to 3 ppm of optically active (N-V) with 8% conversion efficiency. However, a broadening of the (N-V)− zero phonon line was observed in all samples.