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New Journal of Physics

NV center creation in diamond by local CW laser irradiation of shallow implantednitrogen

Alexius Enke, Nicole Raatz, J Meijer, Ralf Wunderlich

Published Jan 13, 2025• 0 citations
Publisher

Abstract

Abstract A novel creation procedure for the nitrogen-vacancy center in diamond is investigated. After shallow nitrogen implantation, a continuous-wave laser is used to induce NV formation, while simultaneously exciting fluorescence to enable live observation. Our investigations imply that a different mechanism than heat induced vacancy diffusion causes the formation of NV centers with this method and we suggest possible alternative pathways which could be responsible, based on the observed properties. Furthermore, we test the procedure for its capabilities for the controlled creation of single centers and show that the emergence of individual centers can be tracked, while achieving sub-micrometer spatial precision.

DOI
10.1088/1367-2630/ada97d

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SPIE Quantum Technologies•Jun 3, 2022•0 citations
Abstract A novel creation procedure for the nitrogen-vacancy center in diamond is investigated. After shallow nitrogen implantation, a continuous-wave laser is used to induce NV formation, while simultaneously exciting fluorescence to enable live observation. Our investigations imply that a different mechanism than heat induced vacancy diffusion causes the formation of NV centers with this method and we suggest possible alternative pathways which could be responsible, based on the observed properties. Furthermore, we test the procedure for its capabilities for the controlled creation of single centers and show that the emergence of individual centers can be tracked, while achieving sub-micrometer spatial precision.
Abstract A novel creation procedure for the nitrogen-vacancy (NV) center in diamond is investigated. After shallow nitrogen implantation, a continuous-wave laser is used to induce NV formation, while simultaneously exciting fluorescence to enable live observation. Our investigations imply that a different mechanism than heat induced vacancy diffusion causes the formation of NV centers with this method and we suggest possible alternative pathways which could be responsible, based on the observed properties. Furthermore, we test the procedure for its capabilities for the controlled creation of single centers and show that the emergence of individual centers can be tracked, while achieving sub-micrometer spatial precision.
Abstract Negatively charged nitrogen‐vacancy (NV − ) centers in diamond are appealing for quantum sensing applications due to their environmental sensitivity and long coherence times. Precise and scalable shallow color center creation is essential yet challenging for technological quantum applications. This is due to the involvement of several lengthy processes, such as ion implantation and thermal annealing of the samples. The latter process can be addressed by application of an alternative activation technique that bypasses the high‐temperature annealing. For this, nitrogen‐implanted regions on a diamond substrate are exposed to continuous‐wave 405 nm laser radiation. The illumination leads to local activation of NV − centers with photoluminescence yield saturation for regions activated with laser power at around 800 µW. For low implantation doses, single NV − centers are created with corresponding mean T 2 coherence time value around 71 µs. The NV − creation yield for the lower implantation doses match conventional creation methods, while higher doses show reduced yield values. However, the coherent properties are comparable to NV − centers within annealed samples. This shows that the activated NV − centers are well‐suited for advanced applications in quantum sensing and related technologies.
Precise control over the spatial distribution and charge state of nitrogen-vacancy (NV) centers in diamond is a key requirement for further advancing this platform in quantum sensing and photonic applications. Here, we investigate nitrogen ion implantation as a scalable method to engineer NV centers in bulk single-crystalline (SC) and a 5 μ m -thick polycrystalline (PC) diamond membrane. Nitrogen-doped regions (1–80 ppm) were fabricated using a 0.7 MeV ion beam and high-temperature annealing, with NV center formation verified by confocal fluorescence imaging and spectral analysis. In SC bulk diamond, we estimate the NV concentration from spectral analysis and model the fluorescence response as a function of implantation dose, capturing both the initial increase at low concentrations and a saturation behavior at higher doses due to quenching mechanisms. In contrast, PC diamond membranes show a weaker dependence at low implantation fluences, consistent with pre-existing nitrogen impurities, thus making a statistical model significantly more complex. The activation yield is found to be of order of 1%, which is lower than in N-rich diamond samples, as implanted N is predominantly interstitial. Photoluminescence spectroscopy indicates that NV 0 is the dominant charge state in both materials, with a laser-power-dependent redistribution between neutral and negative charge states. Optically detected magnetic resonance (ODMR) measurements in SC bulk diamond resolve the hyperfine structure and allow extraction of the dephasing time ( T 2 ∗ ), while in PC diamond membranes, where NV centers tend do form near the grain boundaries, the ODMR signals are observed but spectral resolution is currently limited by impurities, grain-dependent NV orientations, and photoluminescence background.
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.
Laser-induced fluorescence quenching in nitrogen-vacancy (NV) centers in diamond is studied simultaneously with in situ measurements of the heating-induced shift of the electron spin resonance of NV centers in the presence of a microwave field. These experiments reveal a strong correlation between fluorescence suppression in NV centers and the rise of the local temperature inside the diamond crystal. This finding sheds light on quantum pathways behind stimulated fluorescence quenching in NV centers of diamond and may imply significant limitations on the applications of this effect as a method of superresolving imaging in biological systems.
The negatively charged nitrogen-vacancy (NV) center in diamond is among the most promising solid-state systems implementations of a quantum bit. However, integration of the NV center into any efficient photonic environment requires microstructuring the diamond at below-micrometer scale. Preserving the low NV zero-phonon line inhomogeneous broadening during this process is a major challenge with standard NV creation methods. This issue severely limits practical applications of NV centers. Initial studies on pulsed-laser assisted creation of NVs yielded promising results by creating NVs with low inhomogeneous broadening at desired spatial locations in diamond [1]. Crucially, the lattice damage resulting from implantation of energetic ions was avoided. However, the method relied on a narrow window of parameters for successful writing. We widen this window by using a solid immersion lens (SIL), which facilitates laser writing over a broad range of pulse energies and allows for vacancy formation close to a diamond surface without inducing surface graphitization. We operate in the previously unexplored regime where lattice vacancies are created following tunneling breakdown rather than multiphoton ionization [2]. We present NV arrays that have been created between 1 and 40 µm from a diamond surface, all presenting optical linewidth distributions with means as low as 61.0±22.8 MHz [2], including spectral diffusion induced by off-resonant repump for charge stabilization. This emphasizes the exceptionally low charge-noise environment of laser-written NVs. Such high-quality NV centers are excellent candidates for practical applications employing two-photon quantum interference with separate NV centers. Finally, we propose a model for disentangling power broadening from inhomogeneous broadening in the NV zero-phonon line optical linewidth [2]. [1] Y.-C. Chen, P. S. Salter, S. Knauer, … and J. M. Smith, Nat. Photonics 11, 77 (2017). [2] V. Yurgens, J.A Zuber, S. Flågan, M. De Luca, B.J. Shields, I. Zardo, P. Maletinsky, R.J. Warburton, and T. Jakubczyk, ACS Photonics 8, 1726–1734 (2021)