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Biophotonics Australasia

The effect of nitrogen concentration on quantum sensing with nitrogen-vacancy centres

Marco Capelli, Hiroshi Abe, Takeshi Ohshima, Brett C. Johnson, David Simpson, Jan Jeske, Andrew D. Greentree, Philipp Reineck, Brant C. Gibson

Published Dec 30, 2019• 0 citations
Publisher

Abstract

The nitrogen-vacancy (NV) centre in diamond is a perfect candidate for quantum sensing applications applied to numerous fields of science. Past studies improved the sensitivity of diamonds containing NV centres by increasing their density or prolonging their coherence time. However, few studies discussed the effects of other defects inside the diamond crystal on the sensitivity of the NV centres. In this study, we demonstrated the implication of single substitutional nitrogen defects on the fluorescence emission, charge state stability, coherence time and sensitivity of the NV centres. We found that there is an optimal concentration of nitrogen defects that allows diamond samples to have a high-density of NV centres and high fluorescence without significantly affecting the coherence time. This results will inform the correct choice of diamond characteristics for current and future quantum sensing applications with the NV centres.

DOI
10.1117/12.2541225

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The nitrogen-vacancy (NV) centre in diamond is a perfect candidate for quantum sensing applications applied to numerous fields of science. Past studies improved the sensitivity of diamonds containing NV centres by increasing their density or prolonging their coherence time. However, few studies discussed the effects of other defects inside the diamond crystal on the sensitivity of the NV centres. In this study, we demonstrated the implication of single substitutional nitrogen defects on the fluorescence emission, charge state stability, coherence time and sensitivity of the NV centres. We found that there is an optimal concentration of nitrogen defects that allows diamond samples to have a high-density of NV centres and high fluorescence without significantly affecting the coherence time. This results will inform the correct choice of diamond characteristics for current and future quantum sensing applications with the NV centres.
The nitrogen-vacancy (NV) centre in diamond is a perfect candidate for quantum sensing applications applied to numerous fields of science. Past studies improved the sensitivity of diamonds containing NV centres by increasing their density or prolonging their coherence time. However, few studies discussed the effects of other defects inside the diamond crystal on the sensitivity of the NV centres. In this study, we demonstrated the implication of single substitutional nitrogen defects on the fluorescence emission, charge state stability, coherence time and sensitivity of the NV centres. We found that there is an optimal concentration of nitrogen defects that allows diamond samples to have a high-density of NV centres and high fluorescence without significantly affecting the coherence time. This results will inform the correct choice of diamond characteristics for current and future quantum sensing applications with the NV centres.
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.
Abstract The nitrogen-vacancy colour centre in diamond is emerging as one of the most important solid-state quantum systems. It has applications to fields including high-precision sensing, quantum computing, single photon communication, metrology, nanoscale magnetic imaging and biosensing. For all of these applications, a high quantum yield of emitted photons is desirable. However, diamond samples engineered to have high densities of nitrogen-vacancy centres show levels of brightness varying significantly within single batches, or even within the same sample. Here we show that nearby nitrogen impurities quench emission of nitrogen-vacancy centres via non-radiative transitions, resulting in a reduced fluorescence quantum yield. We monitored the emission properties of nitrogen-vacancy centre ensembles from synthetic diamond samples with different concentrations of nitrogen impurities. All samples were irradiated with high energy electrons to create high densities of nitrogen-vacancy centres relative to the concentration of nitrogen impurities. While at low nitrogen densities of 1.81 ppm we measured a lifetime of 13.9 ns, we observed a strong reduction in lifetime with increasing nitrogen density. We measure a lifetime as low as 4.4 ns at a nitrogen density of 380 ppm. The change in lifetime matches a reduction in relative fluorescence quantum yield from 77.4% to 32% with an increase in nitrogen density from 88 ppm to 380 ppm, respectively. These results will inform the conditions required to optimise the properties of diamond crystals devices based on the fluorescence of nitrogen-vacancy centres. Furthermore, this work provides insights into the origin of inhomogeneities observed in high-density nitrogen-vacancy ensembles within diamonds and nanodiamonds.
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 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.
When the word diamond comes up, the majority of people thinks about engagement rings or gemstones. In fact, it is additionally, one of the most promising host materials for the implementation of advanced technology, exploiting the nature of quantum physics. Such quantum technologies have disruptive potential, ones the quantum effects can be applied in macroscopic, commercial products. The nitrogen-vacancy (NV) centre in diamond is a promising candidate to perform such tasks in the fields of quantum computation, quantum cryptography or metrology. Especially in the field of quantum sensing, the NV sensor impresses with nano-scale spatial resolution paired with high sensitivity. The electronic spin of the atomic-sized point defect can be initialised, manipulated and read-out at ambient conditions and coherence lifetimes are comparably long. Diamond magnetometers based on negatively charged NV centres have shown to be very attractive, and the sensitivity goes down to the single-atom level. In order to exploit such a high sensitivity level for sensing prospects, in this thesis, the NV centres are fabricated well confined in a certain distance to the diamond surface, since the detectable field usually decays with the third power of the distance between sensor and target. The surface depicts a fracture of the spin wise protecting diamond lattice and charge fluctuations affect the stability of NV centres, which are overcome by diamond surface termination. In order to improve the sensitivity further, the sensor density, measurement contrast and interaction time are increased. The nitrogen doping technique, which is applied during a plasma-enhanced chemical vapour deposition (PECVD) diamond growth process is used to fabricate NV centre ensembles aligned along one diamond crystal axis, thereby improving the measurement contrast by a factor up to four. The interaction time limiting spin bath is analysed using the sensor capabilities of the NVs, which leads to enhanced growth strategies and the fabrication of sensitivity optimised NV centre ensembles for magnetometry applications.