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physica status solidi (a)

NV‐Center Formation in Single Crystal Diamond at Different CVD Growth Conditions

Mikhail Aleksandrovich Lobaev, А. М. Горбачев, Sergey Aleksandrovich Bogdanov, Anatoly Leontievich Vikharev, Dmitry Borisovich Radishev, Vladimir Aleksandrovich Isaev, Mikhail Nikolaevich Drozdov

Published Sep 24, 2018• 27 citations
Publisher

Abstract

The nitrogen incorporation, diamond growth rate and fluorescence of as‐grown NV centers is studied at different CVD diamond growth conditions. Also, the influence of the misorientation angle is investigated. Heavily nitrogen doped layers are grown at different gas pressures and methane contents, with the maximum nitrogen concentration in the doped layer reaching 7 × 1019 cm−3. The ratio of NV center concentration to the total nitrogen content was determined. The studies are aimed to determine the conditions for creating ensembles with a high concentration of NV centers localized in diamond with nanometer accuracy.

DOI
10.1002/pssa.201800205

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The nitrogen incorporation, diamond growth rate and fluorescence of as‐grown NV centers is studied at different CVD diamond growth conditions. Also, the influence of the misorientation angle is investigated. Heavily nitrogen doped layers are grown at different gas pressures and methane contents, with the maximum nitrogen concentration in the doped layer reaching 7 × 1019 cm−3. The ratio of NV center concentration to the total nitrogen content was determined. The studies are aimed to determine the conditions for creating ensembles with a high concentration of NV centers localized in diamond with nanometer accuracy.
Abstract The nitrogen-vacancy (NV) center in diamond is a promising quantum system for magnetometry applications exhibiting optical readout of minute energy shifts in its spin sub-levels. Key material requirements for NV ensembles are a high NV − concentration, a long spin coherence time and a stable charge state. However, these are interdependent and can be difficult to optimize during diamond growth and subsequent NV creation. In this work, we systematically investigate the NV center formation and properties in bulk chemical vapor deposition (CVD) diamond. The nitrogen flow during growth is varied by over four orders of magnitude, resulting in a broad range of single substitutional nitrogen concentrations of 0.2–20 parts per million. For a fixed nitrogen concentration, we optimize electron-irradiation fluences with two different accelerated electron energies, and we study defect formation via optical characterizations. We discuss a general approach to determine the optimal irradiation conditions, for which an enhanced NV concentration and an optimum of NV charge states can both be satisfied. We achieve spin–spin coherence times T 2 ranging from 45.5 to 549 μ s for CVD diamonds containing 168 to 1 parts per billion NV − centers, respectively. This study shows a pathway to engineer properties of NV-doped CVD diamonds for improved sensitivity.
We systematically investigate the NV center creation and properties in bulk chemical vapor deposition (CVD) diamond, throughout growth, electron-beam irradiation, and annealing steps. We study diamond series grown with a varying nitrogen flow over 4 orders of magnitude, resulting in a broad range of single substitutional nitrogen (P1 center) densities from 0.2 to 20 ppm. We investigate in-situ P1 and NV creations, as well as NV charge states distributions. As the next step, we optimize electron-irradiation fluences for a fixed nitrogen concentration, with two different accelerated electron energies. We bring up a general approach to determine the optimal irradiation conditions, and discuss criteria for P1 to NV conversion ratios in the context of stable NV charge states. Through all these optimizations, we enhance the NV- concentration remarkably in our CVD diamond samples, without sacrificing their Hahn-echo coherence time T2. We achieve NV concentrations from 1 to 168 ppb with T2 from 549 to 45.5 µs respectively. This study shows a pathway to engineer targeted, optimized properties of NV-ensembles in bulk CVD diamonds for improved sensitivity.
Abstract The negatively charged nitrogen vacancy (NV−) center ensemble in as-grown chemical vapor deposition (CVD) diamond is a promising candidate for quantum sensing due to its long coherence time and excellent optical properties. However, achieving a high concentration of NV− centers in as-grown CVD diamond remains a critical challenge, which constrains the performance of NV− based sensors. In this study, we observe that NV− center formation efficiency is significantly enhanced during the initial growth phase, with a coherence time T 2 * of 1.1 μs. These findings demonstrate that high-concentration NV− centers can be achieved in as-grown diamonds, greatly enhancing their utility in high-performance magnetometers and quantum sensing.
Abstract The results of growing multilayered nitrogen-doped nanostructures that have the form of periodically arranged nanometer-thick nitrogen-containing layers in a single-crystal CVD diamond are presented. The possibility of creating nitrogen-doped diamond layers with extremely sharp boundaries (less than 1 nm) is demonstrated. The photoluminescence study have shown that multilayered structures make it possible to obtain a higher radiation intensity of practically important NV – sites at a spin coherence time close to that for uniformly doped layers with the same concentration of nitrogen.
Nitrogen-vacancy (NV) centers in single-crystal CVD diamond are promising candidates for quantum sensing due to their remarkable optical and spin properties [1]. These defects exhibit stable photoluminescence (PL), long spin coherence times, and high sensitivity to external fields [2]. In this study, we present a room-temperature PL characterization of NV centers excited with a 532 nm laser. The setup was optimized for high signal-to-noise ratio and spectral resolution. Key parameters analyzed include emission intensity, zero-phonon line (ZPL) at ~637 nm, phonon sidebands, and the charge state distribution between NV⁰ and NV⁻. The NV⁻ state, crucial for spin-based sensing, is evaluated to understand its stability under different nitrogen doping conditions [3]. The relative intensities of NV⁰ and NV⁻ provide insights into nitrogen incorporation and vacancy formation. These results contribute to optimizing synthesis conditions for enhanced NV⁻ concentration, supporting the advancement of diamond-based quantum sensing technologies.
We report the formation of perfectly aligned, high-density, shallow nitrogen vacancy (NV) centers on the (111) surface of a diamond. The study involved step-flow growth with a high flux of nitrogen during chemical vapor deposition (CVD) growth, which resulted in the formation of a highly concentrated (>1019 cm−3) nitrogen layer approximately 10 nm away from the substrate surface. Photon counts obtained from the NV centers indicated the presence of 6.1 × 1015–3.1 × 1016 cm−3 NV centers, which suggested the formation of an ensemble of NV centers. The optically detected magnetic resonance (ODMR) spectrum confirmed perfect alignment (more than 99%) for all the samples fabricated by step-flow growth via CVD. Perfectly aligned shallow ensemble NV centers indicated a high Rabi contrast of approximately 30% which is comparable to the values reported for a single NV center. Nanoscale nuclear magnetic resonance demonstrated surface-sensitive nuclear spin detection and provided a confirmation of the NV centers' depth. Single NV center approximation indicated that the depth of the NV centers was approximately 9–10.7 nm from the surface with error of less than ±0.8 nm. Thus, a route for material control of shallow NV centers has been developed by step-flow growth using a CVD system. Our finding pioneers on the atomic level control of NV center alignment for large area quantum magnetometry.