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Enhancement of the creation yield of NV ensembles in a chemically vapour deposited diamond

Priyadharshini Balasubramanian, Christian Osterkamp, Ovidiu Brinza, Maxime Rollo, Isabelle Robert-Philip, Philippe Goldner, V. Jacques, Fedor Jelezko, Jocelyn Achard, Alexandre Tallaire

Published Apr 4, 2022• 35 citations
Publisher
DOI
10.1016/j.carbon.2022.04.005

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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.
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.