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Spectrally stable near-surface implanted nitrogen vacancy centers in diamond and the role of surface proximity

Srivatsa Chakravarthi, Christian Pederson, Zeeshawn Kazi, A. D. Ivanov, Kai‐Mei C. Fu

Published May 20, 2021• 0 citations
OpenAlex

Abstract

Scalable realizations of quantum network technologies utilizing the nitrogen vacancy center in diamond require creation of optically coherent NV centers in close proximity to a surface for coupling to optical structures. We create single NV centers by $^{15}$N ion implantation and high-temperature vacuum annealing. Origin of the NV centers is established by optically detected magnetic resonance spectroscopy for nitrogen isotope identification. Near lifetime-limited optical linewidths ($<$ 60 MHz) are observed for the majority of the normal-implant (7$^\circ$, $\approx$ 100 nm deep) $^{15}$NV centers. Long-term stability of the NV$^-$ charge state and emission frequency is demonstrated. The effect of NV-surface interaction is investigated by varying the implantation angle for a fixed ion-energy, and thus lattice damage profile. In contrast to the normal implant condition, NVs from an oblique-implant (85$^\circ$, $\approx$ 20 nm deep) exhibit substantially reduced optical coherence. Our results imply that the surface is a larger source of perturbation than implantation damage for shallow implanted NVs. This work supports the viability of ion implantation for formation of optically stable NV centers. However, careful surface preparation will be necessary for scalable defect engineering.

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Diamond and Related Materials•Sep 12, 2026•0 citations
Scalable realizations of quantum network technologies utilizing the nitrogen vacancy center in diamond require creation of optically coherent NV centers in close proximity to a surface for coupling to optical structures. We create single NV centers by 15^{15}15N ion implantation and high-temperature vacuum annealing. Origin of the NV centers is established by optically detected magnetic resonance spectroscopy for nitrogen isotope identification. Near lifetime-limited optical linewidths (<<< 60 MHz) are observed for the majority of the normal-implant (7∘^\circ∘, ≈\approx≈ 100 nm deep) 15^{15}15NV centers. Long-term stability of the NV−^-− charge state and emission frequency is demonstrated. The effect of NV-surface interaction is investigated by varying the implantation angle for a fixed ion-energy, and thus lattice damage profile. In contrast to the normal implant condition, NVs from an oblique-implant (85∘^\circ∘, ≈\approx≈ 20 nm deep) exhibit substantially reduced optical coherence. Our results imply that the surface is a larger source of perturbation than implantation damage for shallow implanted NVs. This work supports the viability of ion implantation for formation of optically stable NV centers. However, careful surface preparation will be necessary for scalable defect engineering.
Scalable realizations of quantum network technologies utilizing the nitrogen-vacancy (NV) center in diamond require creation of optically coherent NV centers in close proximity to a surface for coupling to optical structures. We create single NV centers by 15N^{15}\mathrm{N}15N ion implantation and high-temperature vacuum annealing. The origin of the NV centers is established by optically detected magnetic resonance spectroscopy for nitrogen isotope identification. Near-lifetime-limited optical linewidths (<60MHz)(<60 \mathrm{MHz})(<60MHz) are observed for the majority of the normal-implant (${7}^{\ensuremath{\circ}}$, $\ensuremath{\approx}100$ nm deep) 15NV^{15}\mathrm{NV}15NV centers. Long-term stability of the ${\mathrm{NV}}^{\ensuremath{-}}$ charge state and emission frequency is demonstrated. The effect of NV-surface interaction is investigated by varying the implantation angle for a fixed ion energy, and thus lattice damage profile. In contrast to the normal-implant condition, NVs from an oblique implant (${85}^{\ensuremath{\circ}}$, $\ensuremath{\approx}20$ nm deep) exhibit substantially reduced optical coherence. Our results imply that the surface is a larger source of perturbation than implantation damage for shallow implanted NVs. This work supports the viability of ion implantation for formation of optically stable NV centers. However, careful surface preparation will be necessary for scalable defect engineering.
We report the observation of stable optical transitions in nitrogen-vacancy (NV) centers created by ion implantation. Using a combination of high temperature annealing and subsequent surface treatment, we reproducibly create NV centers with zero-phonon lines (ZPL) exhibiting spectral diffusion that is close to the lifetime-limited optical line width. The residual spectral diffusion is further reduced by using resonant optical pumping to maintain the NV(-) charge state. This approach allows for placement of NV centers with excellent optical coherence in a well-defined device layer, which is a crucial step in the development of diamond-based devices for quantum optics, nanophotonics, and quantum information science.
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.
Efficient creation of shallow NV−^-− ensembles by high-angle ion implantation
Negatively charged nitrogen-vacancy (NV−^-−) centers located a few nanometers below the diamond surface are key quantum defects for nanoscale sensing of external spins. However, the creation of shallow NV−^-− centers with high yield remains a materials challenge. Here, we demonstrate that high-angle ion implantation enhances the creation efficiency of shallow NV−^-− centers. By implanting 15^{15}15N ions at angles exceeding 60∘^\circ∘, we achieve high NV−^-− yields approaching 10% with effective NV−^-− depths below 10 nm. These yields are significantly higher than those typically reported for shallow NV−^-− creation. The enhanced NV−^-− yield is consistent with an increased vacancy-to-nitrogen ratio in the near-surface region, which is expected to promote NV formation during annealing. The created NV−^-− ensembles show coherence properties comparable to those of single shallow NV−^-− centers at similar depths, and allow detection of nuclear spins in van der Waals materials attached to the diamond surface. Our results establish geometric control of ion implantation as a simple and broadly applicable approach to engineer shallow vacancy-related quantum defects.
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.