We investigated spin-echo coherence times T2 of negatively charged nitrogen vacancy center (NV−) ensembles in single-crystalline diamond synthesized by either the high-pressure and high-temperature and chemical vapor deposition methods. This study specifically examined the magnetic dipole–dipole interaction (DDI) from the various electronic spin baths, which are the source of T2 decoherence. Diamond samples with NV− center concentration [NV−] comparable to those of neutral substitutional nitrogen concentration [Ns0] were used for DDI estimation. Results show that the T2 of the ensemble NV− center decreased in inverse proportion to the concentration of nitrogen-related paramagnetic defects [NPM], being the sum of [Ns0], [NV−], and [NV0], which is a neutrally charged state NV center. This inversely proportional relation between T2 and [NPM] indicates that the nitrogen-related paramagnetic defects of three kinds are the main decoherence source of the ensemble NV− center in the single-crystalline diamond. We found that the DDI coefficient of NVH− center was significantly smaller than that of Ns0, the NV0 center, or the NV− center. We ascertained the DDI coefficient of the NV− center DNV− through experimentation using a linear summation of the decoherence rates of each nitrogen-related paramagnetic defect. The obtained value of 89 μs ppm for DNV− corresponds well to the value estimated from the relation between DDI coefficient and spin multiplicity.
We investigated spin-echo coherence times T2 of negatively charged nitrogen vacancy center (NV−) ensembles in single-crystalline diamond synthesized by either the high-pressure and high-temperature and chemical vapor deposition methods. This study specifically examined the magnetic dipole–dipole interaction (DDI) from the various electronic spin baths, which are the source of T2 decoherence. Diamond samples with NV− center concentration [NV−] comparable to those of neutral substitutional nitrogen concentration [Ns0] were used for DDI estimation. Results show that the T2 of the ensemble NV− center decreased in inverse proportion to the concentration of nitrogen-related paramagnetic defects [NPM], being the sum of [Ns0], [NV−], and [NV0], which is a neutrally charged state NV center. This inversely proportional relation between T2 and [NPM] indicates that the nitrogen-related paramagnetic defects of three kinds are the main decoherence source of the ensemble NV− center in the single-crystalline diamond. We found that the DDI coefficient of NVH− center was significantly smaller than that of Ns0, the NV0 center, or the NV− center. We ascertained the DDI coefficient of the NV− center DNV− through experimentation using a linear summation of the decoherence rates of each nitrogen-related paramagnetic defect. The obtained value of 89 μs ppm for DNV− corresponds well to the value estimated from the relation between DDI coefficient and spin multiplicity.
Nitrogen doped diamond single crystals grown using either HPHT synthesis or CVD method were examined. After the diamond growth, electron beam irradiation and post annealing at 1000℃ for 2h were carried out to form NV-centers in the diamond crystals. For creating NV- center whose amount is comparable to that of neutral substitutional nitrogen Ns0, the total fluences of electron beam was set in the range of 1×1017 to 1×1018 e/cm-2. The 1/T2 can be expressed as summation of 1/T2{Ns0}, 1/T2{NV-} and T2{NV0}.2 By removing of the relaxation rate from Ns0 and NV0 center from 1/T2, we obtained the inverse relationship between T2{NV-} and [NV-] as shown in figure. The inverse relationship shows that DDI between NV centers is successfully detected. It is clarified that strength of DDI from NV- center: DNV- is about twice as large as those of Ns0 and NV0 center.2 It is expected that the large strength of DDI leads to shorten T2 with increasing of [NV-].
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.
Because of their high sensitivity, quantum materials are extremely promising for new technologies. The main challenge lies in maintaining a sufficiently quantum coherence times for quantum computation or quantum sensing systems. NV centers in diamond which are point defects consisting of a substitutional nitrogen atom neighboring an atomic vacancy, where an electron pair can reside in a triplet state – are ideal candidates for the development of industrial-scale quantum systems. These spin states exhibit ms-long coherence times at room temperature and can be manipulated optically, hence opening interesting perspectives for sending magnetic fields with high sensitivity1.At HiQuTe Diamond, we take up the challenge of mastering the entire nitrogen-doped diamond production chain synthesized by Microwave Plasma-Assisted Chemical Vapor Deposition (MPACVD). We aim at creating affordable diamonds specially engineered to achieve long coherence times with high NV density and high doping uniformity. This quest require to overcome the impact of several external factors that contribute to electron spin decoherence. First, the chemical composition of the diamond, specifically the types and concentrations of impurities within the diamond matrix (such as substitutional nitrogen NS, NV centres, mono-vacancies and clusters, hydrogen, etc.), as well as their electrical charge states (NS⁰, NS⁺, NV⁰, NV⁻) should be carefully controlled. Thanks to extensive scientific research conducted over the past decade, combined with our own R&D efforts, we are now able to quantify these parameters using experimental techniques compatible with industrial applications (Raman and UV-Vis spectroscopy) and compare our results with key performance indicators2. Second, we study the relationship between coherence (T2*) and strain inhomogeneities in our diamond layers, which we analyse using birefringence measurements. Our findings demonstrate our capability to produce CVD diamond layers with reduced strain and extended defect and confirm that strain could be a critical limiting factor for T2*.In this poster, I will review the efforts carried out at HiQuTe Diamond to develop specific material that is well suited for quantum sensing applications.References1.Barry, J. F., Schloss, J. M., Bauch, E., Turner, M. J., Hart, C. A., Pham, L. M., & Walsworth, R. L. (2020). Sensitivity optimization for NV-diamond magnetometry. Reviews of Modern Physics, 92(1), 015004.2.Langer, J. (2022). Quantum-grade diamond for cavity-based solutions. Fraunhofer Verlag.
Abstract Nitrogen-vacancy (NV) centers in diamond have been developed into essential hardware units for a wide range of solid-state-based quantum technology applications. While such applications require the long spin coherence times of the NV centers, they are often limited due to decoherence. In this study, we theoretically investigate the decoherence of NV-spin ensembles induced by nitrogen impurities (P1 centers), which are one of the most dominant and inevitable magnetic field noise sources in diamond. We combined cluster correlation expansion and density functional theory to compute the Hahn-echo spin-coherence time of the NV centers for a broad range of P1 concentrations. Results indicate a clear linear dependence of T2 on P1 concentrations on a log scale with a slope of −1.06, which is in excellent agreement with previous experimental results. The interplay between the Jahn–Teller effect and the hyperfine interaction in the P1 center plays a critical role in determining the bath dynamics and the resulting NV decoherence. Our results provide a theoretical upper bound for the NV-spin T2 over a wide range of P1 densities, serving as a key reference for materials optimization and spin bath characterization to develop highly coherent NV-based devices for quantum information technology.
To improve the sensitivity of magnetic sensors using negatively charged nitrogen-vacancy (NV−) centers, it is essential to improve the quality of diamond crystals and precisely control the nitrogen concentration in the crystals. We have utilized high-pressure, high-temperature synthesis [1] and chemical vapor deposition [2] for the growth of nitrogen-doped diamond. The concentration of substitutional nitrogen in the neutral charge state [NS0] were evaluated by electron paramagnetic resonance (EPR) measurements. As shown in Fig. 1, [NS0] were precisely controlled by the weight ratio of nitrogen getter material in the metal solvent for the HPHT method (Fig. 1(a)) and by the carbon to nitrogen gas ratio for the CVD method (Fig. 1(b)). Then, the diamond crystals were irradiated with electron beams followed by vacuum annealing so that 10% of the nitrogen at the substitutional site became NV− centers, and the negatively charged NV− centers were successfully formed preferentially [3]. T2 of these diamond crystals was inversely proportional to the nitrogen concentration. The product of T2 and nitrogen concentration of the obtained HPHT diamond crystal is slightly higher than the maximum value reported so far [4], suggesting that the crystal is expected to have high magnetic sensitivity.
Ensembles of nitrogen-vacancy (NV) centers in diamond are versatile quantum sensors with broad applications in the physical and life sciences. The concentration of neutral substitutional nitrogen ( [ N s 0 ]) strongly influences NV electronic spin coherence times, sensitivity, and optimal sensing strategies. Diamonds with [ N s 0 ] ∼ 1–10 ppm are a focus of recent material engineering efforts, with higher concentrations being favorable for continuous-wave optically detected magnetic resonance (CW-ODMR) and lower concentrations expected to benefit pulsed magnetometry techniques through extended NV spin coherence times and improved sensing duty cycles. In this work, we synthesize and characterize low- [ N s 0 ] ( ∼ 0.8 ppm), NV-enriched diamond material, engineered through low-strain chemical vapor deposition (CVD) growth on high-quality substrates, 12 C isotopic purification, and controlled electron irradiation and annealing. Our results demonstrate good strain homogeneity in diamonds grown on CVD substrates and spin-bath-limited NV dephasing times. By measuring NV spin and charge properties across a wide range of optical NV excitation intensity, we provide direct comparisons of photon-shot-noise-limited magnetic field sensitivity between the current low- [ N s 0 ] and previously studied higher- [ N s 0 ] ( ∼ 14 ppm) NV-diamond sensors. We show that low- [ N s 0 ] diamond can outperform higher- [ N s 0 ] diamond at moderate and low optical NV excitation intensity. Our results provide practical benchmarks and guidance for selecting NV-diamond sensors tailored to specific experimental constraints and sensing requirements.