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Charge stability of shallow single nitrogen-vacancy centers in lightly boron-doped diamond

Taisuke Kageura, Yosuke Sasama, Chikara Shinei, Tokuyuki Teraji, K. Yamada, Shinobu Onoda, Takahide Yamaguchi

Published Jan 14, 2022• 17 citations
Publisher
DOI
10.1016/j.carbon.2022.01.027

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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.

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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.
A nitridation process of a diamond surface with nitrogen radical exposure far from the radio-frequency plasma for the stabilization of a negatively charged nitrogen-vacancy (NV − ) centers near the surface is presented. At a nitrogen coverage of as high as 0.9 monolayers, high average Rabi contrasts of 0.40 ± 0.06 and 0.46 ± 0.03 have been obtained for single NV − centers formed by shallow nitrogen implantation with acceleration voltages of 1 and 2 keV, respectively. This indicates that nitrogen termination by a radical exposure process produces an electric charge state suitable for single NV − centers near the surface compared with the states obtained for alternatively terminated surfaces.
This is a preliminary version. Improvements and additional analysis will be included in a revised manuscript. We investigate the charge-state stability of individual nitrogen-vacancy (NV) centers in weakly doped HPHT IIa diamond containing sub-ppm concentrations of boron and nitrogen. Using Ti/Al coplanar electrodes on an oxygen-terminated surface, we study how applied electric fields and optical excitation jointly govern NV charge conversion. By combining voltage-dependent photoluminescence, real-time charge-state monitoring, laser-power saturation with spectral decomposition, and time-resolved measurements, we reveal that electric fields several micrometers from the contacts significantly increase the NV- population and enhance spin readout. At low excitation powers, the NV- population evolves on minute timescales following compressed-exponential kinetics, consistent with slow space-charge rearrangement in ultra-insulating diamond. Under pulsed excitation, we observe hundreds-of-nanoseconds NV-/NV0 conversion driven by hole capture, which is strongly suppressed by applied bias. Our results demonstrate that residual boron acceptors play a key role in determining charge-state stability and show how electrical bias can reliably stabilize NV- in weakly doped bulk diamond.