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arXiv:2208.12706 · physica status solidi (RRL) - Rapid Research Letters

The Study of the Efficiency of Nitrogen to Nitrogen‐Vacancy (NV)‐Center Conversion in High‐Nitrogen Content Samples

Stepan V. Bolshedvorskii, Сергей Александрович Тарелкин, Vladimir V. Soshenko, I. S. Cojocaru, Olga R. Rubinas, Vadim N. Sorokin, Victor G. Vins, Andrey N. Smolyaninov, С.Г. Буга, Artem S. Galkin, Т. Е. Дроздова, Mikhail S. Kuznetsov, S.A. Nosukhin, Alexey V. Akimov

Published Dec 14, 2022• 7 citations
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Abstract

The nitrogen‐vacancy color center in diamond is one of the important systems in the fast‐growing field of sensing. This color center is used in both high‐resolution and high‐sensitivity sensors. However, techniques for the quick and efficient formation of NV centers are still in the development stage. Herein, a study on the influence of the electron irradiation dose on the conversion of substitutional nitrogen into NV− centers is presented. The study is done on diamonds that are highly enriched with nitrogen (≈100 ppm), which, on one hand, should maximize the effect of irradiation, and, on other hand, be of interest for high‐sensitivity magnetometers. The maximum achieved conversion efficiency is as high as 37% ± 3.7%, with no observed saturation on the electron dose even with the simplest annealing procedure. The measurements of the corresponding dephasing time made it possible to make a theoretical estimate for the shot‐noise‐limited magnetic field sensitivity per unit volume of diamond to be roughly .

DOI
10.1002/pssr.202200415

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The nitrogen‐vacancy color center in diamond is one of the important systems in the fast‐growing field of sensing. This color center is used in both high‐resolution and high‐sensitivity sensors. However, techniques for the quick and efficient formation of NV centers are still in the development stage. Herein, a study on the influence of the electron irradiation dose on the conversion of substitutional nitrogen into NV− centers is presented. The study is done on diamonds that are highly enriched with nitrogen (≈100 ppm), which, on one hand, should maximize the effect of irradiation, and, on other hand, be of interest for high‐sensitivity magnetometers. The maximum achieved conversion efficiency is as high as 37% ± 3.7%, with no observed saturation on the electron dose even with the simplest annealing procedure. The measurements of the corresponding dephasing time made it possible to make a theoretical estimate for the shot‐noise‐limited magnetic field sensitivity per unit volume of diamond to be roughly .
The sensitivity of the nitrogen-vacancy (NV) color centers in diamond-based magnetometers strongly depends on the number of NV centers involved in the measurement. Unfortunately, an increasing concentration of NV centers leads to a decrease in their dephasing and coherence times if the nitrogen content exceeds a certain threshold level (approximately 1017cm-3 or 0.6 ppm). Here, we demonstrate that this increased dephasing can be efficiently compensated for by optimizing the electron irradiation dose in postprocessing procedures in the vicinity of the threshold concentration, thus extending the range of possible useful concentrations of NV centers in diamonds with a natural carbon content.
The negatively charged nitrogen−vacancy (NV − ) center ensembles in diamonds offer enormous potential for developing integrated sensors with an improved signal-to-noise ratio (SNR) and high sensitivity. However, the preparation and treatment of diamond samples with suitable NV − concentrations and dephasing time have remained challenging. This work provided insight into the NV − center formation mechanism and reconstruction via a comprehensive analysis of the concentration and dephasing time of a set of diamond samples treated by various parameters. By varying the electron irradiation dose and subsequent annealing duration, the conversion rate of nitrogen to NV − is up to 18.45%, and the corresponding maximum NV − concentration is 3.69 ppm. The dephasing time for all samples varies around 300 ns. The nitrogen-related NV − center ensemble dephasing rate per unit density is 146.4 (ppm·ms) −1 , indicating that the treatment did not substantially alter the paramagnetic spin environment around the NV − center. This study not only offers support to exquisite sensitivities of NV-based sensors but also provides valuable experience for the preparation of unique properties of synthetic diamonds.
NV- center has been paid attention as a quantum sensor for highly sensitive detection of magnetic field, electric field, temperature and strain, etc.. Electron beam irradiation followed by subsequent thermal annealing is known as the effective procedures to create NV- center in diamond. The electron irradiation generates vacancies in diamond and the annealing enables vacancies to diffuse in the lattice. Then diffused vacancies are captured by nitrogen atoms, and as a result, NV centers are created. In addition, substitutional nitrogen atom at a lattice site (P1 center) also acts as a donor for NV center, the charge state of NV centers changes from neutral (NV0) to NV-. Creation high concentration of ensemble NV- centers is needed to achieve high sensitively sensing. The magnetic sensitivity is proportional to the reciprocal of the number of NV centers and T2 (spin coherence time), i.e., high concentration NV- centers with long T2 increase the sensitivity. P1 center has an important role for being a component of NV- centers and acting as donor to the NV center. But it also plays a role as decoherence source (decrease in magnetic field sensitivity). Therefore, it is important to create high concentration of NV- centers considering the amount of P1 centers. In current study, we investigate irradiation fluence dependence of the creation behavior of NV centers in type-Ib diamonds by using electron spin resonance (ESR) and photo-luminescence (PL) to understand the creation mechanism of NV- center. The values of T2 are also evaluated by Hahn-echo measurement, since it is one of the key parameters for highly sensitive magnetometry. Then, we discuss the creation mechanism of NV centers based on concentrations of defects.
The nitrogen vacancy (NV) center in diamond has been well applied in quantum sensing of electromagnetic field and temperature, where the sensitivity can be enhanced by the number of NV centers. Here, we used electron beam irradiation to increase the generation rate of NV centers by nearly 22 times. We systematically studied the optical and electronic properties of the NV center as a function of an electron irradiation dose, where the detection sensitivity of magnetic fields was improved. With such samples with dense NV centers, a sub-pico-Tesla sensitivity in magnetic fields detection can be achieved with optimal controls and detections.
The dynamics of the formation of ensembles of nitrogen–vacancy color centers (NV centers) in single-crystal diamond plates after irradiation by high-energy (2 MeV) electrons and subsequent annealing is investigated. The concentration of the nitrogen impurity is determined from the infrared (IR) absorption spectrum to be 90 and 4 ppm for the diamond growth sectors {111} and {001}, respectively. The transverse relaxation times T2∗T_{2}^{*}T2∗​ for the electron spin of NV centers are studied; they are found to amount to 200 and 900 ns for the {111} and {001} sectors, respectively, and are limited by the concentration of paramagnetic impurity defects in diamond. The sensitivity of quantum sensors based on the obtained ensembles of NV centers is estimated; the estimation shows feasibility of using denser ensembles in low-field magnetometry.
The studies of many-body dynamics of interacting spin ensembles, as well as quantum sensing in solid state systems, are often limited by the need for high spin concentrations, along with efficient decoupling of the spin ensemble from its environment. In particular, for an ensemble of nitrogen-vacancy (NV) centers in diamond, high conversion efficiencies between nitrogen (P1) defects and NV centers are essential while maintaining long coherence times of an NV ensemble. In this work, we study the effect of electron irradiation on the conversion efficiency and the coherence time of various types of diamond samples with different initial nitrogen concentrations. The samples were irradiated using a 200 keV transmission electron microscope. Our study reveals that the efficiency of NV creation strongly depends on the initial conversion efficiency and on the initial nitrogen concentration. The irradiation of the examined samples exhibits an order of magnitude improvement in the NV concentration (up to ∼1011 NV/cm2), without degradation in their coherence time of ∼180 μs. We address the potential of this technique toward the study of many-body physics of NV ensembles and the creation of non-classical spin states for quantum sensing.