Abstract The properties and creation of optical centers in diamond are essential for applications in quantum technology. Here, we study the photoluminescence (PL) spectroscopy behavior at low temperatures of diamond subjected to electron irradiation and annealing heat treatment. Through temperature variation testing, it was found that the NV − center intensity of diamond with a nitrogen content of 150 ppm before treatment is insensitive to the experimental temperature, but significantly increases with decreasing temperature after treatment, showing sensitivity to temperature. In addition, the H3 center also shows an increasing trend with decreasing temperature. The results of annealing diamond with a nitrogen content of 730 ppm showed that even at a low temperature of 93 K, no NV − centers were detected, but there were a large number of Ni-N related centers, especially NE8 centers. Our findings can promote a deeper understanding of the behavioral characteristics of HPHT-diamond optical centers in low-temperature environments.
Abstract The properties and creation of optical centers in diamond are essential for applications in quantum technology. Here, we study the photoluminescence (PL) spectroscopy behavior at low temperatures of diamond subjected to electron irradiation and annealing heat treatment. Through temperature variation testing, it was found that the NV − center intensity of diamond with a nitrogen content of 150 ppm before treatment is insensitive to the experimental temperature, but significantly increases with decreasing temperature after treatment, showing sensitivity to temperature. In addition, the H3 center also shows an increasing trend with decreasing temperature. The results of annealing diamond with a nitrogen content of 730 ppm showed that even at a low temperature of 93 K, no NV − centers were detected, but there were a large number of Ni-N related centers, especially NE8 centers. Our findings can promote a deeper understanding of the behavioral characteristics of HPHT-diamond optical centers in low-temperature environments.
Electron irradiation is one of the most powerful methods to create negatively charged nitrogen-vacancy centers (NV-s) in diamonds, which act as qubits and quantum sensors even at room temperature (RT). For quantum sensing, it is important to create ensemble NV-s with long coherence time (T2) since the sensitivity can be affected by both amount of NV- and T2. For high concentration NV-, electron irradiation with higher fluence is needed. However, if electron fluence is too high, neutral NVs (NV0s) are created because of lack of N donors. For T2, since residual defects act as origins of T2 decoherence, it is important to optimize the condition of subsequent annealing as well as irradiation fluence. Thus, we need to consider initial nitrogen (P1) concentration in diamond, electron fluence, and annealing conditions. In this paper, we create NV-s in Ib diamonds by electron irradiation and subsequent annealing with different conditions, and study the amounts of NV-s and their T2 for high-sensitive quantum sensing. The samples used in this study were Ib diamond with P1 concentration around 100 ppm. Those samples were irradiated with 2 MeV-electrons at a fluence of 1x1018/cm2 at RT. After irradiation, the samples were annealed between 600 and 1400oC in Ar. Photoluminescence (PL) measurements were carried out at RT to confirm NV creation. For PL measurements, the laser with a wavelength of 532 nm was used as excitation. PL intensity for samples annealed at 600 oC is about half even after annealing for 600 min, comparing with that for 800 oC-annealed samples although the values increase with increasing annealing time. Thus, the annealing at 650 oC is not enough to create NV. The samples annealed between 800 and 1200 oC show the highest PL intensity even after annealing for 10 min. The 800 and 1000 oC-annealed samples keep the PL intensity after annealing for 1200 min although the PL intensity for 1200 oC-annealed samples decrease with increasing annealing time above 100 min. The PL intensity for the samples annealed at 1400 oC shows smaller value and decreases with increasing annealing time. For T2, the samples annealed at 1400 oC show 2 microsec after annealing for 10 min. However, NV- cannot be observed after annealing at 1400 oC for 30min. Therefore, it can be concluded that annealing at 1400 oC is not suitable for the creation of NV-. For samples annealed between 600 and 1000 oC, the values of T2 are constant (between 0.5 and 0.9 microsec) after annealing up to 1200 min. For samples annealed at 1200 oC, no significant difference in T2 value is observed from those annealed between 600 and 1000 oC up to 30min, and the value increases with increasing annealing time above 30 min. From the point of view of sensing, it is important to consider both the amounts of NV- centers and T2. Therefore, we compare the values of PL intensity times T2. As a result, the samples annealed between 800 and 1200 oC show the highest value although the value for samples annealed at 1200 oC decreases after annealing for 1200 min. This suggests that annealing at 800 oC for 10 min is enough to create NV-s. We also study the creation of NV-s in diamonds by electron irradiation at elevated temperature. The samples with P1 concentration around 60 and 100 ppm were irradiated with 2 MeV-electrons at fluences up to 5x1018/cm2 at 800 or 1000 oC. The samples were annealed at 1000 oC for 120 min after irradiation. The amounts of NV are estimated from electron spin resonance (ESR) signals. As a result, samples irradiated at 800 and 1000 oC show higher NV- concentration than that for RT-irradiated ones, and 800 oC-irradiated ones show higher NV concentration than 1000oC-irradiated ones. Since the T2 values are not affected by irradiation temperature, the elevated temperature irradiation, especially 800 oC irradiation is a useful method to realize quantum sensing with high sensitivity.
Quantum information applications place stringent demands on the development of platforms that can host them. Color centers in diamond have been identified as important media for quantum information processing. Accordingly, the photoluminescence properties of nitrogen-vacancy (N-V) centers in diamond created by implantation and annealing are studied at cryogenic temperatures (below 10 K). We examine high pressure high temperature and chemical vapor deposition synthetic diamonds with varying nitrogen concentration and present an accurate method to estimate the concentration of the (N-V) centers created by ion implantation. The ion irradiation route produced up to 6 ppm of optically active (N-V) centers, while nitrogen implantation yielded up to 3 ppm of optically active (N-V) with 8% conversion efficiency. However, a broadening of the (N-V)− zero phonon line was observed in all samples.
Abstract We report an investigation of spectral and temporal properties of NV¯ centers in diamond plates fabricated from a single HPHT crystal but subjected to different electron irradiation doses during postgrowth processing. Samples 52734-1 and 52734-2, each with approximately the same nitrogen concentration of 60 ppm, are irradiated with doses of 1 and 2 × 1018 e‒/cm2, respectively. Particular attention is paid to the effect of irradiation dose on the concentration of NV¯ centers and the associated changes in the spectral and temporal properties of superluminescence under identical conditions of optical excitation with laser radiation at a wavelength of 532 nm. Analysis of the absorption spectra reveals that doubling the irradiation dose results in a 1.4-fold increase in the concentration of NV¯ centers—from 7.7 to 10.9 ppm—with a corresponding decrease in the concentration of isolated nitrogen centers (C centers)—from 49 to 43 ppm. The results demonstrate a nonlinear dependence of the increase in the concentration of NV¯ centers on the irradiation dose and make it possible to identify key characteristics of the samples and pumping conditions that determine the efficiency of superluminescence. Specifically, doubling the irradiation dose results in a threefold increase in the spectral intensity and a significant decrease in the duration of the superluminescence pulses. It is found that to achieve efficient superluminescence, it is important not only to have a significant excess of the concentration of C centers over the concentration of NV¯ centers, but also the absolute concentration of NV¯ centers and pump parameters such as the energy density of the pump pulses and the volume of the sample with a population inversion.
Abstract In the context of the NV− diamond laser creation [1], an urgent task is to determine the characteristics of diamonds that can affect the laser generation. This work is aimed at investigating the mechanisms of the creation of superluminescence in diamond under the action of optical pumping by the second harmonic of the Nd:YAG laser (λ = 532nm). It was found that when the HPHT diamond is irradiated by 532 nm radiation with an intensity above ~ 2.0 MW/cm2, a nonlinear intensity increasing in the spectral region 700–750 nm is manifested against the background of the spontaneous photoluminescence spectrum, which, with a further pumping intensity increasing turns into a pronounced peak of superluminescence with a maximum of about 718 nm. An increase in the pumping intensity from 2.7 to 46 MW/cm2 widened this peak at half-maximum from 13 to 19 nm. At high levels of pumping intensity, nonlinear pumping radiation absorption and accumulation of NV centers in the excited state were detected. The position of the photoluminescence band was calculated depending on different values of the population inversion density of the color centers, taking into account the diamond's own absorption spectrum. The calculation results are close to the experimental data.
The negatively-charged nitrogen-vacancy (NV) center is the most studied optical center in diamond and is very important for applications in quantum information science. Many proposals for integrating NV centers in quantum and sensing applications rely on their tailored fabrication in ultra pure host material. In this study, we use ion implantation to controllably introduce nitrogen into high purity, low nitrogen chemical vapor deposition diamond samples. The properties of the resulting NV centers are studied as a function of implantation temperature, annealing temperature, and implantation fluence. We compare the implanted NV centers with native NV centers present deep in the bulk of the as-grown samples. The results for implanted NV centers are promising but indicate, at this stage, that the deep native NV centers possess overall superior optical properties. In particular, the implanted NV centers obtained after annealing at 2000 °C under a stabilizing pressure of 8 GPa showed an ensemble linewidth of 0.17 nm compared to 0.61 nm after annealing at 1000 °C. Over the same temperature range, the ensemble NV−/NV0 ratio increased by a factor of ∼5, although this was accompanied by an overall decrease in the NV count.
Negatively charged nitrogen-vacancy (NV-) center in diamond has been paid attention as a highly sensitive detector for magnetic field. The magnetic sensitivity is proportional to the reciprocal of √(NT_2 ), where N is the number of NV centers and T2 is the spin coherence time. To improve the sensitivity, high concentration of NV- centers and extended coherence time are necessary. It is generally known that electron beam irradiation into type-Ib diamond which include high initial concentration of isolated substitutional nitrogen (P1 center) is a useful method to create high concentration of NV- centers. The electron beam irradiation generates vacancies in diamond and the subsequently annealing enables vacancies to diffuse in the lattice. Then diffused vacancies are captured by nitrogen atoms, as a result, NV centers are created. The post annealing has been performed at 1000°C or higher temperature for the purpose of improving the spin properties of NV- centers. In current study, we focused on post-annealing at high temperature to improve magnetic sensitivity of quantum sensing. We investigated annealing temperature and time dependence of the creation behavior of NV centers in type-Ib diamonds to understand appropriate annealing process for enhancing sensitivity of NV- center.