Shallow, negatively-charged Nitrogen-Vacancy centers (NV-) in diamond have been proposed for high-sensitivity magnetometry and spin-polarization transfer applications. However, surface effects tend to favor and stabilize the less useful neutral form, the NV0 centers. Here, we report the effects of green laser irradiation on ensembles of nanometer-shallow NV centers in flat and nanostructured diamond surfaces as a function of laser power in a range not previously explored (up to 150 mW/μm2). Raman spectroscopy, optically-detected-magnetic-resonance (ODMR) and charge-photoconversion fluorescence detection are applied to characterize the properties and dynamics of NV- and NV0 centers. We demonstrate that high laser power strongly promotes photoconversion of NV0 to NV- centers. Surprisingly, the excess NV- population is stable over a time scale of one hundred milliseconds after switching off the laser, resulting in long-lived enrichment of shallow NV-. The beneficial effect of photoconversion is less marked in nanostructured samples. Our results are important to inform the design of samples and experimental procedures for applications relying on ensembles of shallow NV- centers in diamond.
Shallow, negatively-charged Nitrogen-Vacancy centers (NV-) in diamond have been proposed for high-sensitivity magnetometry and spin-polarization transfer applications. However, surface effects tend to favor and stabilize the less useful neutral form, the NV0 centers. Here, we report the effects of green laser irradiation on ensembles of nanometer-shallow NV centers in flat and nanostructured diamond surfaces as a function of laser power in a range not previously explored (up to 150 mW/μm2). Raman spectroscopy, optically-detected-magnetic-resonance (ODMR) and charge-photoconversion fluorescence detection are applied to characterize the properties and dynamics of NV- and NV0 centers. We demonstrate that high laser power strongly promotes photoconversion of NV0 to NV- centers. Surprisingly, the excess NV- population is stable over a time scale of one hundred milliseconds after switching off the laser, resulting in long-lived enrichment of shallow NV-. The beneficial effect of photoconversion is less marked in nanostructured samples. Our results are important to inform the design of samples and experimental procedures for applications relying on ensembles of shallow NV- centers in diamond.
Shallow, negatively charged nitrogen-vacancy centers (NV -) in diamond have been proposed for high-sensitivity magnetometry and spin-polarization transfer applications.However, surface effects tend to favor and stabilize the less useful neutral form, the NV 0 centers.Here, we report the effects of green laser irradiation on ensembles of nanometer-shallow NV centers in flat and nanostructured diamond surfaces as a function of laser power in a range not previously explored (up to 150 mW/μm 2 ).Fluorescence spectroscopy, optically detected magnetic resonance (ODMR), and charge-photoconversion detection are applied to characterize the properties and dynamics of NV -and NV 0 centers.We demonstrate that high laser power strongly promotes photoconversion of NV 0 to NV -centers.Surprisingly, the excess NV -population is stable over a timescale of 100 ms after switching off the laser, resulting in long-lived enrichment of shallow NV -.The beneficial effect of photoconversion is less marked in nanostructured samples.Our results are important to inform the design of samples and experimental procedures for applications relying on ensembles of shallow NV -centers in diamond.
Negatively charged nitrogen-vacancy (NV−) centers in diamond have unique magneto-optical properties, such as high fluorescence, single-photon generation, millisecond-long coherence times, and the ability to initialize and read the spin state using purely optical means. This makes NV− centers a powerful sensing tool for a range of applications, including magnetometry, electrometry, and thermometry. Biocompatible NV-rich nanodiamonds find application in cellular microscopy, nanoscopy, and in vivo imaging. NV− centers can also detect electron spins, paramagnetic agents, and nuclear spins. Techniques have been developed to hyperpolarize 14N, 15N, and 13C nuclear spins, which could open up new perspectives in NMR and MRI. However, defects on the diamond surface, such as hydrogen, vacancies, and trapping states, can reduce the stability of NV− in favor of the neutral form (NV0), which lacks the same properties. Laser irradiation can also lead to charge-state switching and a reduction in the number of NV− centers. Efforts have been made to improve stability through diamond substrate doping, proper annealing and surface termination, laser irradiation, and electric or electrochemical tuning of the surface potential. This article discusses advances in the stabilization and enrichment of shallow NV− ensembles, describing strategies for improving the quality of diamond devices for sensing and spin-polarization transfer applications. Selected applications in the field of biosensing are discussed in more depth.
As promising quantum sensors, nitrogen-vacancy (N-V) centers in diamond have been widely used in frontier studies in condensed-matter physics, material science, and life sciences. In practical applications, weak laser excitation is favorable as it reduces the side effects of laser irradiation, such as phototoxicity and heating. Here we report a combined theoretical and experimental study of (near) zero-field optically detected magnetic resonance (ODMR) of N-V-center ensembles under weak 532-nm laser excitation. In this region, both the width and splitting of the ODMR spectra decrease with increasing laser power. This power dependence is reproduced with a model that accounts for the laser-induced charge neutralization of $\mathrm{N}\text{\ensuremath{-}}{V}^{\ensuremath{-}}$--N+ pairs, which alters the local electric field environment. These results are useful for the understanding and development of N-V-based quantum sensing in light-sensitive applications.
Nitrogen vacancy (NV) centers in diamond have been identified over the past few years as promising systems for a variety of applications, ranging from quantum information science to magnetic sensing. This relies on the unique optical and spin properties of the negatively charged NV. Many of these applications require shallow NV centers, i.e., NVs that are close (a few nm) to the diamond surface. In recent years there has been increasing interest in understanding the spin and charge dynamics of NV centers under various illumination conditions, specifically under infrared (IR) excitation, which has been demonstrated to have significant impact on the NV centers' emission and charge state. Nevertheless, a full understanding of all experimental data is still lacking, with further complications arising from potential differences between the photodynamics of bulk and shallow NVs. Here we suggest a generalized quantitative model for NV center spin- and charge-state dynamics under both green and IR excitation. We experimentally extract the relevant transition rates, providing a comprehensive model which reconciles all existing experimental results in the literature, except for highly nonlinear regimes. Moreover, we identify key differences between the photodynamics of bulk and shallow NVs, and use them to significantly enhance the initialization fidelity of shallow NVs to the useful negatively charged state.
The nitrogen-vacancy (NV) centers in diamond have the advantages of stable triaxial structure, ultra-long electron spin coherence time and simple optical readout at room temperature. A nitrogen atom in the diamond crystal replaces a carbon atom and a vacancy is generated at the adjacent position, forming a point defect in the C3v space group structure. Its ground state and excited state are both spin triplet states. It is the key to achieving efficient preparation of optical initial state and extracting NV color center’s information in the researches of highly sensitive sensing magnetic detection, temperature detection, biological imaging, quantum computing, etc. However, there was no systematic study on relevant parameters of laser for high-concentration NV color center’s samples in previous experimental studies. Based on a high concentration diamond NV ensemble, we use pulsed optical detection magnetic resonance (ODMR) technology to systematically study the relationship among laser initial polarization time, information reading time and laser power, and the influence of laser incident polarization angle on the accuracy of sensing information. The effects of various laser parameters on the NV1 peak of ODMR on the [111] axis of the NVs of diamond are also investigated. The contrast of ODMR increases firstly with a sigmoid function and then decreases with an e-exponential function as the information reading time increases. The incident polarization angle of the laser is sinusoidal, with a period of 90°. According to the above experimental results, we finally choose the appropriate experimental parameters at 45.8 W/cm2 (300 μs of polarization, 700 ns, reading time, laser incident angle is 220°) for ODMR test. Compared with previous experimental parameters (polarization time was 50 us, read the time of 3000 ns, laser incident angle was 250°), the experimental results show that the contrast of ODMR increases from 2.1% to 4.6%, and the typical magnetic sensitivity is improved from 21.6 nT/Hz1/2 to 5.6 nT/Hz1/2. The optimization of the optical control of NVs in solid diamond is realized. The above results provide an effective support for the detection of high-sensitivity manipulation sensing based on high-concentration NV ensemble.
We created dense ensembles of negatively charged nitrogen-vacancy (NV-) centers in diamond by neutron and electron irradiation for applications in hybrid quantum systems and magnetometry. We characterize fluorescence intensity, optical and coherence properties of the resulting defects by confocal microscopy, UV/Vis and FTIR spectroscopy, optically detected magnetic resonance and small angle X-ray scattering. We find the highest densities of NV- at neutron fluences on the order of 10^17 cm^-2 and electron doses of 10^18 cm^-2, with spin resonance linewidths of 6 MHz. Lower electron energies increase the ratio of centers in the desired negative charge state to those in the neutral one. Annealing at 900 °C during the irradiation reduces the spin resonance linewidth. Electron irradiation furthermore results in substantially higher optical transparency compared to neutron irradiation.