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arXiv:1206.4260 · Applied Physics Letters

Long coherence time of spin qubits in 12C enriched polycrystalline chemical vapor deposition diamond

K. D. Jahnke, B. Naydenov, T. Teraji, S. Koizumi, T. Umeda, J. Isoya, Fedor Jelezko

Published Jul 2, 2012• 67 citations
arXivHTMLPDF

Abstract

Single defects in diamond and especially negatively charged nitrogen vacancy (NV) centers are very promising quantum systems with wide applications in physics and biology. It was shown that their coherence properties can be strongly improved by growing ultrapure diamond with low concentration of parasitic spins associated with nitrogen electron spins and nuclear spins related to $^{13}$C carbon isotope. Here we report a high quality $^{12}$C-enriched polycrystalline CVD diamond material with properties comparable with single crystals. We find single NVs in the grains of this material, which show extremely long electron spin coherence time $T_2 > 2\,ms$.

DOI
10.1063/1.4731778

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Single defects in diamond and especially negatively charged nitrogen vacancy (NV) centers are very promising quantum systems with wide applications in physics and biology. It was shown that their coherence properties can be strongly improved by growing ultrapure diamond with low concentration of parasitic spins associated with nitrogen electron spins and nuclear spins related to 13^{13}13C carbon isotope. Here we report a high quality 12^{12}12C-enriched polycrystalline CVD diamond material with properties comparable with single crystals. We find single NVs in the grains of this material, which show extremely long electron spin coherence time T2>2 msT_2 > 2\,msT2​>2ms.
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.
Spins of negatively charged nitrogen-vacancy (NV${}^{\ensuremath{-}}$) defects in diamond are among the most promising candidates for solid-state qubits. The fabrication of quantum devices containing these spin-carrying defects requires position-controlled introduction of NV${}^{\ensuremath{-}}$ defects having excellent properties such as spectral stability, a long spin coherence time, and a stable negative charge state. Nitrogen ion implantation and annealing enable the positioning of NV${}^{\ensuremath{-}}$ spin qubits with high precision, but to date, the coherence times of qubits produced this way are short, presumably because of the presence of residual radiation damage. In the present work, we demonstrate that a high-temperature annealing at 1000 ${}^{\ensuremath{\circ}}$C allows 2 ms coherence times to be achieved at room temperature. These results were obtained for implantation-produced NV${}^{\ensuremath{-}}$ defects in a high-purity, 99.99% 12{}^{12}12C-enriched single crystal chemical vapor deposited diamond. We discuss these long coherence times in the context of the thermal behavior of residual defect spins.
Fluorescent nanodiamonds (FNDs) containing negatively charged nitrogen-vacancy (NV-) centers are vital for many emerging quantum sensing applications from magnetometry to intracellular sensing in biology. However, developing a scalable fabrication method for FNDs hosting color centers with consistent bulk-like photoluminescence (PL) and spin coherence properties remains a highly desired but unrealized goal. Here, we investigate optimized ball milling of single-crystal diamonds produced via chemical vapor deposition (CVD) and containing 2 ppm of substitutional nitrogen and 0.3 ppm of NV- to achieve this goal. The NV charge state, PL lifetime, and spin properties of bulk CVD diamond samples are directly compared to milled CVD FNDs and commercial high-pressure high-temperature (HPHT) FNDs. We find that on average, the relative contribution of the NV- charge state to the total NV PL is lower and the NV PL lifetime is longer in CVD FNDs compared to HPHT FNDs, both likely due to the lower Ns0 concentration in CVD FNDs. The CVD bulk and CVD FNDs on average show similar average T1 spin relaxation times of 3.2 ±\pm± 0.7 ms and 4.7 ±\pm± 1.6 ms, respectively, compared to 0.17 ±\pm± 0.01 ms for commercial HPHT FNDs. Our results demonstrate that ball milling of CVD diamonds enables the large-scale fabrication of NV ensembles in FNDs with bulk-like T1 spin relaxation properties.
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 Diamond hosts a wide variety of colour centres that have demonstrated outstanding optical and spin properties. Among them, the nitrogen-vacancy (NV) centre is by far the most investigated owing to its superior characteristics, which promise the development of highly sophisticated quantum devices, in particular for sensing applications. Nevertheless, harnessing the potential of these centres mainly relies on the availability of high quality and purity diamond single crystals that need to be specially designed and engineered for this purpose. Plasma assisted chemical vapour deposition (CVD) has become a key enabling technology in this field of research. Nitrogen can indeed be directly doped in situ into a high crystalline quality diamond matrix in a controlled way, allowing the production of single isolated centres or ensembles that can potentially be integrated into a device. In this paper we will provide an overview of the requirements for synthesizing ‘quantum-grade’ diamond films using CVD. These include the reduction of impurities and surrounding spins that limit coherence times, the control of NV density in a wide range of concentrations as well as their spatial localization within the diamond. Enhancing the charge state and preferential orientation of the colour centres is also discussed. These improvements in material fabrication have contributed to positioning diamond as one of the most promising solid-state quantum systems and the first industrial applications in sensing are just starting to emerge.
Abstract Fluorescent nanodiamonds (FNDs) containing negatively charged nitrogen-vacancy (NV − ) centers are vital for many emerging quantum sensing applications from magnetometry to intracellular sensing in biology. However, developing a scalable fabrication method for FNDs hosting color centers with consistent bulk-like photoluminescence (PL) and spin coherence properties remains a highly desired but unrealized goal. Here, we investigate optimized ball milling of single-crystal diamonds produced via chemical vapor deposition (CVD) and containing 2 ppm of substitutional nitrogen and 0.3 ppm of NV − to achieve this goal. The NV charge state, PL lifetime, and spin properties of bulk CVD diamond samples are directly compared to milled CVD FNDs and commercial high-pressure high-temperature (HPHT) FNDs. We find that on average, the relative contribution of the NV − charge state to the total NV PL is lower and the NV PL lifetime is longer in CVD FNDs compared to HPHT FNDs, both likely due to the lower N s 0 concentration in CVD FNDs. The CVD bulk and CVD FNDs on average show similar average T 1 spin relaxation times of 3.2 ± 0.7 ms and 4.7 ± 1.6 ms, respectively, compared to 0.17 ± 0.01 ms for commercial HPHT FNDs. Our results demonstrate that ball milling of CVD diamonds enables the large-scale fabrication of NV ensembles in FNDs with bulk-like T 1 spin relaxation properties.