arXiv:2303.08091 · Philosophical Transactions of the Royal Society A Mathematical Physical and Engineering Sciences
Absorption and birefringence study for reduced optical losses in diamond with high nitrogen-vacancy concentration
Tingpeng Luo, Felix A. Hahl, Julia Langer, V. Cimalla, Lukas Lindner, Xavier Vidal, Marko Haertelt, Rémi Blinder, Shinobu Onoda, Takeshi Ohshima, Jan Jeske
The use of diamond colour centres such as the nitrogen-vacancy (NV) centre is increasingly enabling quantum sensing and computing applications. Novel concepts like cavity coupling and readout, laser-threshold magnetometry and multi-pass geometries allow significantly improved sensitivity and performance via increased signals and strong light fields. Enabling material properties for these techniques and their further improvements are low optical material losses via optical absorption of signal light and low birefringence. Here, we study systematically the behaviour of absorption around 700 nm and birefringence with increasing nitrogen- and NV-doping, as well as their behaviour during NV creation via diamond growth, electron beam irradiation and annealing treatments. Absorption correlates with increased nitrogen doping yet substitutional nitrogen does not seem to be the direct absorber. Birefringence reduces with increasing nitrogen doping. We identify multiple crystal defect concentrations via absorption spectroscopy and their changes during the material processing steps and thus identify potential causes of absorption and birefringence as well as strategies to fabricate chemical vapour deposition diamonds with high NV density yet low absorption and low birefringence. This article is part of the Theo Murphy meeting issue 'Diamond for quantum applications'.
The use of diamond colour centres such as the nitrogen-vacancy (NV) centre is increasingly enabling quantum sensing and computing applications. Novel concepts like cavity coupling and readout, laser-threshold magnetometry and multi-pass geometries allow significantly improved sensitivity and performance via increased signals and strong light fields. Enabling material properties for these techniques and their further improvements are low optical material losses via optical absorption of signal light and low birefringence. Here, we study systematically the behaviour of absorption around 700 nm and birefringence with increasing nitrogen- and NV-doping, as well as their behaviour during NV creation via diamond growth, electron beam irradiation and annealing treatments. Absorption correlates with increased nitrogen doping yet substitutional nitrogen does not seem to be the direct absorber. Birefringence reduces with increasing nitrogen doping. We identify multiple crystal defect concentrations via absorption spectroscopy and their changes during the material processing steps and thus identify potential causes of absorption and birefringence as well as strategies to fabricate chemical vapour deposition diamonds with high NV density yet low absorption and low birefringence. This article is part of the Theo Murphy meeting issue 'Diamond for quantum applications'.
Diamond color centers such as the nitrogen-vacancy (NV) center have been extensively studied as a popular platform that enables quantum sensing and computing applications. For highly sensitive sensing NV ensembles have significantly stronger signals than individual NV centers and can create strong light fields, which are also essentially required by novel concepts that need a large sensing volume, such as cavity coupling and readout, laser threshold magnetometry and multi-pass geometries. On top of strong signals, low optical material losses are the other key consideration for these techniques, by means of low optical absorption of signal light and low birefringence of the diamond crystal. In this work, we study systematically the behavior of absorption in the NV emission range around 700nm and birefringence with increasing nitrogen- and NV-doping, as well as their behavior during NV creation via diamond growth, electron beam irradiation and annealing treatments. Absorption correlates with increased nitrogen-doping yet single substitutional nitrogen atoms (Ns0 or P1 centers) do not seem to be the direct absorber. The high nitrogen doping level in the growth leads to high absorption in the whole UV-Vis range, which is the main contributors to the high absorption at 700 nm. When treating the diamond for an enhanced NV concentration, ‘over irradiating’ the diamond with too high fluence is harmful in the sense of creating neutral vacancies that increase absorption at the wavelength range of interest. Opposite to the absorption, birefringence reduces with increasing nitrogen doping and shows better homogeneity. After-growth treatments show a minor and if any a positive (i.e. reducing) influence on diamond birefringence. Multiple crystal defect concentrations and their changes are identified via absorption spectroscopy during the material processing steps and thus we identify potential causes of absorption and birefringence. From this we suggest strategies to fabricate CVD diamonds with high NV density yet low absorption and low birefringence
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 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.
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.
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.