Abstract Negatively charged nitrogen-vacancy (NV − ) center ensembles in diamond have proved to have great potential for use in highly sensitive, small-package solid-state quantum sensors. One way to improve sensitivity is to produce a high-density NV − center ensemble on a large scale with a long coherence lifetime. In this work, the NV − center ensemble is prepared in type-Ib diamond using high energy electron irradiation and annealing, and the transverse relaxation time of the ensemble— T 2 —was systematically investigated as a function of the irradiation electron dose and annealing time. Dynamical decoupling sequences were used to characterize T 2 . To overcome the problem of low signal-to-noise ratio in T 2 measurement, a coupled strip lines waveguide was used to synchronously manipulate NV − centers along three directions to improve fluorescence signal contrast. Finally, NV − center ensembles with a high concentration of roughly 10 15 mm −3 were manipulated within a ~10 µ s coherence time. By applying a multi-coupled strip-lines waveguide to improve the effective volume of the diamond, a sub-femtotesla sensitivity for AC field magnetometry can be achieved. The long-coherence high-density large-scale NV − center ensemble in diamond means that types of room-temperature micro-sized solid-state quantum sensors with ultra-high sensitivity can be further developed in the near future.
Abstract Negatively charged nitrogen-vacancy (NV − ) center ensembles in diamond have proved to have great potential for use in highly sensitive, small-package solid-state quantum sensors. One way to improve sensitivity is to produce a high-density NV − center ensemble on a large scale with a long coherence lifetime. In this work, the NV − center ensemble is prepared in type-Ib diamond using high energy electron irradiation and annealing, and the transverse relaxation time of the ensemble— T 2 —was systematically investigated as a function of the irradiation electron dose and annealing time. Dynamical decoupling sequences were used to characterize T 2 . To overcome the problem of low signal-to-noise ratio in T 2 measurement, a coupled strip lines waveguide was used to synchronously manipulate NV − centers along three directions to improve fluorescence signal contrast. Finally, NV − center ensembles with a high concentration of roughly 10 15 mm −3 were manipulated within a ~10 µ s coherence time. By applying a multi-coupled strip-lines waveguide to improve the effective volume of the diamond, a sub-femtotesla sensitivity for AC field magnetometry can be achieved. The long-coherence high-density large-scale NV − center ensemble in diamond means that types of room-temperature micro-sized solid-state quantum sensors with ultra-high sensitivity can be further developed in the near future.
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.
The negatively charged nitrogen−vacancy (NV − ) center ensembles in diamonds offer enormous potential for developing integrated sensors with an improved signal-to-noise ratio (SNR) and high sensitivity. However, the preparation and treatment of diamond samples with suitable NV − concentrations and dephasing time have remained challenging. This work provided insight into the NV − center formation mechanism and reconstruction via a comprehensive analysis of the concentration and dephasing time of a set of diamond samples treated by various parameters. By varying the electron irradiation dose and subsequent annealing duration, the conversion rate of nitrogen to NV − is up to 18.45%, and the corresponding maximum NV − concentration is 3.69 ppm. The dephasing time for all samples varies around 300 ns. The nitrogen-related NV − center ensemble dephasing rate per unit density is 146.4 (ppm·ms) −1 , indicating that the treatment did not substantially alter the paramagnetic spin environment around the NV − center. This study not only offers support to exquisite sensitivities of NV-based sensors but also provides valuable experience for the preparation of unique properties of synthetic diamonds.
NV- center has been paid attention as a quantum sensor for highly sensitive detection of magnetic field, electric field, temperature and strain, etc.. Electron beam irradiation followed by subsequent thermal annealing is known as the effective procedures to create NV- center in diamond. The electron irradiation generates vacancies in diamond and the annealing enables vacancies to diffuse in the lattice. Then diffused vacancies are captured by nitrogen atoms, and as a result, NV centers are created. In addition, substitutional nitrogen atom at a lattice site (P1 center) also acts as a donor for NV center, the charge state of NV centers changes from neutral (NV0) to NV-. Creation high concentration of ensemble NV- centers is needed to achieve high sensitively sensing. The magnetic sensitivity is proportional to the reciprocal of the number of NV centers and T2 (spin coherence time), i.e., high concentration NV- centers with long T2 increase the sensitivity. P1 center has an important role for being a component of NV- centers and acting as donor to the NV center. But it also plays a role as decoherence source (decrease in magnetic field sensitivity). Therefore, it is important to create high concentration of NV- centers considering the amount of P1 centers. In current study, we investigate irradiation fluence dependence of the creation behavior of NV centers in type-Ib diamonds by using electron spin resonance (ESR) and photo-luminescence (PL) to understand the creation mechanism of NV- center. The values of T2 are also evaluated by Hahn-echo measurement, since it is one of the key parameters for highly sensitive magnetometry. Then, we discuss the creation mechanism of NV centers based on concentrations of defects.
The studies of many-body dynamics of interacting spin ensembles, as well as quantum sensing in solid state systems, are often limited by the need for high spin concentrations, along with efficient decoupling of the spin ensemble from its environment. In particular, for an ensemble of nitrogen-vacancy (NV) centers in diamond, high conversion efficiencies between nitrogen (P1) defects and NV centers are essential while maintaining long coherence times of an NV ensemble. In this work, we study the effect of electron irradiation on the conversion efficiency and the coherence time of various types of diamond samples with different initial nitrogen concentrations. The samples were irradiated using a 200 keV transmission electron microscope. Our study reveals that the efficiency of NV creation strongly depends on the initial conversion efficiency and on the initial nitrogen concentration. The irradiation of the examined samples exhibits an order of magnitude improvement in the NV concentration (up to ∼1011 NV/cm2), without degradation in their coherence time of ∼180 μs. We address the potential of this technique toward the study of many-body physics of NV ensembles and the creation of non-classical spin states for quantum sensing.
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.
We created dense ensembles of negatively charged nitrogen-vacancy (NV-) centers in diamond by neutron and electron irradiation for applications in hybrid quantum systems and magnetometry. We characterize fluorescence intensity, optical and coherence properties of the resulting defects by confocal microscopy, UV/Vis and FTIR spectroscopy, optically detected magnetic resonance and small angle X-ray scattering. We find the highest densities of NV- at neutron fluences on the order of 10^17 cm^-2 and electron doses of 10^18 cm^-2, with spin resonance linewidths of 6 MHz. Lower electron energies increase the ratio of centers in the desired negative charge state to those in the neutral one. Annealing at 900 °C during the irradiation reduces the spin resonance linewidth. Electron irradiation furthermore results in substantially higher optical transparency compared to neutron irradiation.