Since nitrogen-vacancy (NV) centers in diamond have emerged as crucial quantum sensors in physics and biology, the massive preparation of high-quality and high-concentration shallow NV center samples has become urgent and demanding. As NV centers approach the surface and their concentration increases, charge state instability can degrade coherence and introduce additional noise. This problem is further complicated in high-pressure and high-temperature (HPHT) diamonds due to the presence of unclear impurities and inhomogeneous strain. Through optically detected magnetic resonance testing on various implanted samples, we analyzed the spin and charge state properties of shallow NV center ensembles. Our results reveal that the doping dose significantly influences the quantity of NV−, charge, and charge stability. Our findings indicate that over-implanting nitrogen as electron donors before starting graphitization helps stabilize the charge environment of the shallow NV center ensembles. By controlling the nitrogen ion implantation dose, we optimized charge state stability under photoionization and prepared high-quality NV center ensemble samples in HPHT diamonds at the optimal implantation dose range of 2×1013–8×1013 ions/cm2. This method, which relies solely on nitrogen ion implantation and annealing on HPHT diamond, significantly reduces the cost of sensor samples, greatly benefiting the promotion of quantum sensing.
Since nitrogen-vacancy (NV) centers in diamond have emerged as crucial quantum sensors in physics and biology, the massive preparation of high-quality and high-concentration shallow NV center samples has become urgent and demanding. As NV centers approach the surface and their concentration increases, charge state instability can degrade coherence and introduce additional noise. This problem is further complicated in high-pressure and high-temperature (HPHT) diamonds due to the presence of unclear impurities and inhomogeneous strain. Through optically detected magnetic resonance testing on various implanted samples, we analyzed the spin and charge state properties of shallow NV center ensembles. Our results reveal that the doping dose significantly influences the quantity of NV−, charge, and charge stability. Our findings indicate that over-implanting nitrogen as electron donors before starting graphitization helps stabilize the charge environment of the shallow NV center ensembles. By controlling the nitrogen ion implantation dose, we optimized charge state stability under photoionization and prepared high-quality NV center ensemble samples in HPHT diamonds at the optimal implantation dose range of 2×1013–8×1013 ions/cm2. This method, which relies solely on nitrogen ion implantation and annealing on HPHT diamond, significantly reduces the cost of sensor samples, greatly benefiting the promotion of quantum sensing.
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.
Dense and shallow ensembles of negatively charged nitrogen-vacancy center (NV−) with good optical and spin properties play a key role in the performance enhancement of diamond-based quantum sensors. Ion implantation enables precise control of NV− depth and density. However, at high ion fluence, this method is limited by low NV− creation yields and sample amorphization. Additionally, shallow NV− spin properties deteriorate due to surface proximity. In this paper, we study N2+ ion implantation at energies between 10 and 15 keV with fluences as high as 1×1015 ions/cm2 at temperatures of 20, 400, and 800°C to investigate the influence of implantation temperature on lattice damage, NV− creation yield, and NV− spin properties. Our results show that diamond maintains structural integrity at 800°C with fluences up to 1×1015 ions/cm2 without amorphization. Furthermore, high-temperature implantation improves NV− creation yields up to five times without compromising T2∗, T2, and T1, making it a promising approach to enhance the magnetic field sensitivity of NV− ensembles.
Creating dense and shallow nitrogen-vacancy (NV) ensembles with good spin properties is a prerequisite for developing diamond-based quantum sensors exhibiting better performance. Ion implantation is a key enabling tool for precisely controlling spatial localization and density of NV color centers in diamond. However, it suffers from a low creation yield, while higher ion fluences significantly damage the crystal lattice. In this work, we realize N2+ ion implantation in the 30–40 keV range at high temperatures. At 800 °C, NV's ensemble photoluminescence emission is three to four times higher than room temperature implanted films, while narrow electron spin resonance linewidths of 1.5 MHz, comparable to well-established implantation techniques, are obtained. In addition, we found that ion fluences above 2 × 1014 ions/cm2 can be used without graphitization of the diamond film, in contrast to room temperature implantation. This study opens promising perspectives in optimizing diamond films with implanted NV ensembles that could be integrated into quantum sensing devices.
Enhanced magnetic field sensitivity of shallow NV− ensembles via high-temperature implantation
Dense and shallow ensembles of negatively charged nitrogen-vacancy centers (NV−) with good optical and spin properties play a key role in the performance enhancement of diamond-based quantum sensors. Ion implantation enables precise control of NV− depth and density. However, at high ion fluence, this method is limited by low NV− creation yields and sample amorphization. Additionally, shallow NV− spin properties deteriorate due to surface proximity. In this paper, we study N2+ ion implantation at energies between 10 and 15 keV with fluences as high as 1e15 ions/cm2 at temperatures of 20, 400 and 800°C to investigate the influence of implantation temperature on lattice damage, NV− creation yield and NV− spin properties. Our results show that diamond maintains structural integrity at 800°C with fluences up to 1e15 ions/cm2 without amorphization. Furthermore, high-temperature implantation improves NV− creation yields up to five times without compromising T2∗, T2 and T1, making it a promising approach to enhance the magnetic field sensitivity of NV− ensembles.
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.
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 15N ions at angles exceeding 60∘, 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.