Charge Stability and Charge-State-Based Spin Readout of Shallow Nitrogen-Vacancy Centers in Diamond.

Spin-based applications of the negatively charged nitrogen-vacancy (NV) center in diamonds require an efficient spin readout. One approach is the spin-to-charge conversion (SCC), relying on mapping the spin states onto the neutral (NV0) and negative (NV-) charge states followed by a subsequent charge readout. With high charge-state stability, SCC enables extended measurement times, increasing precision and minimizing noise in the readout compared to the commonly used fluorescence detection. Nanoscale sensing applications, however, require shallow NV centers within a few nanometers distance from the surface where surface related effects might degrade the NV charge state. In this article, we investigate the charge state initialization and stability of single NV centers implanted ≈5 nm below the surface of a flat diamond plate. We demonstrate the SCC protocol on four shallow NV centers suitable for nanoscale sensing, obtaining a reduced readout noise of 5-6 times the spin-projection noise limit. We investigate the general applicability of the SCC for shallow NV centers and observe a correlation between the NV charge-state stability and readout noise. Coating the diamond with glycerol improves both the charge initialization and stability. Our results reveal the influence of the surface-related charge environment on the NV charge properties and motivate further investigations to functionalize the diamond surface with glycerol or other materials for charge-state stabilization and efficient spin-state readout of shallow NV centers suitable for nanoscale sensing.

Indirect overgrowth as a synthesis route for superior diamond nano sensors.

The negatively charged nitrogen-vacancy ([Formula: see text]) center shows excellent spin properties and sensing capabilities on the nanoscale even at room temperature. Shallow implanted [Formula: see text] centers can effectively be protected from surface noise by chemical vapor deposition (CVD) diamond overgrowth, i.e. burying them homogeneously deeper in the crystal. However, the origin of the substantial losses in [Formula: see text] centers after overgrowth remains an open question. Here, we use shallow [Formula: see text] centers to exclude surface etching and identify the passivation reaction of NV to NVH centers during the growth as the most likely reason. Indirect overgrowth featuring low energy (2.5-5 keV) nitrogen ion implantation and CVD diamond growth before the essential annealing step reduces this passivation phenomenon significantly. Furthermore, we find higher nitrogen doses to slow down the NV-NVH conversion kinetics, which gives insight into the sub-surface diffusion of hydrogen in diamond during growth. Finally, nano sensors fabricated by indirect overgrowth combine tremendously enhanced [Formula: see text] and [Formula: see text] times with an outstanding degree of depth-confinement which is not possible by implanting with higher energies alone. Our results improve the understanding of CVD diamond overgrowth and pave the way towards reliable and advanced engineering of shallow [Formula: see text] centers for future quantum sensing devices.

dc Magnetometry with Engineered Nitrogen-Vacancy Spin Ensembles in Diamond.

The exquisite optical and spin properties of nitrogen-vacancy (NV) centers in diamond have made them a promising platform for quantum sensing. The prospect of NV-based sensors relies on the controlled production of these atomic-scale defects. Here we report on the fabrication of a preferentially oriented, shallow ensemble of NV centers and their applicability for sensing dc magnetic fields. For the present sample, the residual paramagnetic impurities are the dominant source of environmental noise, limiting the dephasing time (T2*) of the NVs. By controlling the P1 spin-bath, we achieve a 4-fold improvement in the T2* of the NV ensemble. Further, we show that combining spin-bath control and homonuclear decoupling sequence cancels NV-NV interactions and partially protects the sensors from a broader spin environment, thus extending the ensemble T2* up to 10 µs. With this decoupling protocol, we measure an improved dc magnetic field sensitivity of 1.2 nT µm3/2 Hz-1/2. Using engineered NVs and decoupling protocols, we demonstrate the prospects of harnessing the full potential of NV-based ensemble magnetometry.

Engineering preferentially-aligned nitrogen-vacancy centre ensembles in CVD grown diamond.

Here we report a method for improving the magnetic field sensitivity of an ensemble of Nitrogen-Vacancy (NV) centres in 12C-enriched diamond aligned along the [111] crystal axis. The preferentially-aligned NV centres are fabricated by a Plasma Enhanced Chemical Vapour Deposition (PECVD) process and their concentration is quantitatively determined by analysing the confocal microscopy images. We further observe that annealing the samples at high temperature (1500 °C) in vacuum leads to a conversion of substitutional nitrogen into NV centres. This treatment also increases the coherence time of the NV centres electron spins up to 40 µs, which corresponds to enhancement of the sensitivity by a factor of three. However, this procedure also leads to a loss of the preferential alignment by 34%.

Contributed Review: Camera-limits for wide-field magnetic resonance imaging with a nitrogen-vacancy spin sensor.

Sensitive, real-time optical magnetometry with nitrogen-vacancy centers in diamond relies on accurate imaging of small (≪10-2), fractional fluorescence changes across the diamond sample. We discuss the limitations on magnetic field sensitivity resulting from the limited number of photoelectrons that a camera can record in a given time. Several types of camera sensors are analyzed, and the smallest measurable magnetic field change is estimated for each type. We show that most common sensors are of a limited use in such applications, while certain highly specific cameras allow achieving nanotesla-level sensitivity in 1 s of a combined exposure. Finally, we demonstrate the results obtained with a lock-in camera that paves the way for real-time, wide-field magnetometry at the nanotesla level and with a micrometer resolution.

Toward Optimized Surface δ-Profiles of Nitrogen-Vacancy Centers Activated by Helium Irradiation in Diamond.

The negatively charged nitrogen-vacancy (NV) center in diamond has been shown recently as an excellent sensor for external spins. Nevertheless, their optimum engineering in the near-surface region still requires quantitative knowledge in regard to their activation by vacancy capture during thermal annealing. To this aim, we report on the depth profiles of near-surface helium-induced NV centers (and related helium defects) by step-etching with nanometer resolution. This provides insights into the efficiency of vacancy diffusion and recombination paths concurrent to the formation of NV centers. It was found that the range of efficient formation of NV centers is limited only to approximately 10 to 15 nm (radius) around the initial ion track of irradiating helium atoms. Using this information we demonstrate the fabrication of nanometric-thin (δ) profiles of NV centers for sensing external spins at the diamond surface based on a three-step approach, which comprises (i) nitrogen-doped epitaxial CVD diamond overgrowth, (ii) activation of NV centers by low-energy helium irradiation and thermal annealing, and (iii) controlled layer thinning by low-damage plasma etching. Spin coherence times (Hahn echo) ranging up to 50 µs are demonstrated at depths of less than 5 nm in material with 1.1% of (13)C (depth estimated by spin relaxation (T1) measurements). At the end, the limits of the helium irradiation technique at high ion fluences are also experimentally investigated.