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arXiv:2511.12591

Charge-state stability of single NV centers in HPHT-type IIa diamond

Darya Meniailava, Michael Petrov, Josef Soucek, Milos Nesladek

quant-phSubmitted Nov 16, 2025• Announced Nov 18, 2025• 0 citations• Revised Nov 20, 2025 (v2)
v1 · Nov 16, 2025v2 · Nov 20, 2025
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Abstract

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.

Comments
Draft version. 13 pages, 4 figures. A more complete version will follow

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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.
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.
Abstract Charge state instabilities have been a bottleneck for the implementation of solid-state spin systems and pose a major challenge to the development of spin-based quantum technologies. Here we investigate the stabilization of negatively charged nitrogen-vacancy (NV−) centers in phosphorus-doped diamond at liquid helium temperatures. Photoionization of phosphorous donors in conjunction with charge diffusion at the nanoscale enhances NV0 to NV− conversion and stabilizes the NV− charge state without the need for an additional repump laser. The phosphorus-assisted stabilization is explored and confirmed both with experiments and our theoretical model. Stable photoluminescence-excitation spectra are obtained for NV− centers created during the growth. The fluorescence is continuously recorded under resonant excitation to real-time monitor the charge state and the ionization and recombination rates are extracted from time traces. We find a linear laser power dependence of the recombination rate as opposed to the conventional quadratic dependence, which is attributed to the photo-ionization of phosphorus atoms.
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.
The ability to control the charge and spin states of nitrogen-vacancy (NV) centers near the diamond surface is of pivotal importance for quantum applications. Hydrogen-terminated diamond is promising for long spin coherence times and ease of controlling the charge states due to the low density of surface defects. However, it has so far been challenging to create negatively charged single NV centers with controllable spin states beneath a hydrogen-terminated surface because atmospheric adsorbates that act as acceptors induce surface holes. In this study, we optically detected the magnetic resonance of shallow single NV centers in hydrogen-terminated diamond through precise control of the nitrogen implantation fluence. Furthermore, we found that the probability of detecting the resonance was enhanced by reducing the surface acceptor density through passivation of the hydrogen-terminated surface with hexagonal boron nitride without air exposure. This control method opens up new opportunities for using NV centers in quantum applications.
The charge state stability of nitrogen-vacancy (NV) centers critically affects their application as quantum sensors and qubits. Understanding charge state conversion and equilibration is important not only for NV centers in diamond but also for defects and impurities in wide-bandgap materials in general. The mechanisms by which these centers change charge state upon optical or electronic excitation without the presence of mobile carriers remain unclear. Here, we elucidate this issue for the case of photoionization of NV center ensembles. Using pump-probe spectroscopy, we ionize negatively charged NV centers and monitor the recovery of NV^{-} on timescales of up to several seconds. We find that the recovery rate depends strongly on the concentration of surrounding nitrogen donors. Remarkably, the equilibration dynamics exhibit no discernible dependence on temperature, ruling out thermally activated processes. We develop a multiphonon-assisted electron-tunneling model, supported by density-functional calculations, that explains the measurements and identifies tunneling as the equilibration mechanism. Because tunneling rates depend exponentially on donor separation, the random distribution of nitrogen donors spreads recovery times from nanoseconds to hours or longer.
Charge state instabilities have been a bottleneck for the implementation of solid-state spin systems and pose a major challenge to the development of spin-based quantum technologies. Here we investigate the stabilization of negatively charged nitrogen-vacancy (NV−^-−) centers in phosphorus-doped diamond at liquid helium temperatures. Photoionization of phosphorous donors in conjunction with charge diffusion at the nanoscale enhances NV0^00 to NV−^-− conversion and stabilizes the NV−^-− charge state without the need for an additional repump laser. The phosphorus-assisted stabilization is explored and confirmed both with experiments and our theoretical model. Stable photoluminescence-excitation spectra are obtained for NV−^-− centers created during the growth. The fluorescence is continuously recorded under resonant excitation to real-time monitor the charge state and the ionization and recombination rates are extracted from time traces. We find a linear laser power dependence of the recombination rate as opposed to the conventional quadratic dependence, which is attributed to the photo-ionization of phosphorus atoms.