High-density nitrogen-vacancy (NV) centers exceeding 1016/cm3 inside a diamond can be achieved by femtosecond laser irradiation. The number of pulses and pulse energy were adjusted considering the increasing trend of the NV concentration and damage generation. The NV concentration first grew as the number of laser pulses was increased, and then the concentration was temporarily saturated or decreased. By increasing the number of laser pulses more than 2.5–5 × 107, the concentration increased again. The Hahn-echo measurement revealed that electron spins of the substitutional nitrogen center (P1) were dominant source for decoherence and the number of paramagnetic defects induced by the laser irradiation was not significant for degradation of spin coherence of the laser-induced NV centers even without a post-annealing process. Such high-dense ensemble NV centers are crucial for a high-sensitive quantum sensor.
High-density nitrogen-vacancy (NV) centers exceeding 1016/cm3 inside a diamond can be achieved by femtosecond laser irradiation. The number of pulses and pulse energy were adjusted considering the increasing trend of the NV concentration and damage generation. The NV concentration first grew as the number of laser pulses was increased, and then the concentration was temporarily saturated or decreased. By increasing the number of laser pulses more than 2.5–5 × 107, the concentration increased again. The Hahn-echo measurement revealed that electron spins of the substitutional nitrogen center (P1) were dominant source for decoherence and the number of paramagnetic defects induced by the laser irradiation was not significant for degradation of spin coherence of the laser-induced NV centers even without a post-annealing process. Such high-dense ensemble NV centers are crucial for a high-sensitive quantum sensor.
Nitrogen-vacancy (NV) centers in diamond are expected to be quantum sensing devices such as magnetic and electric fields, temperature, pressure and so on. The generation of NV centers by irradiations of femtosecond laser pulses has been reported. Femtosecond laser can write NV centers in diamond directly and this direct writing can realize a flexible spatial arrangement of NV centers. As the application of the laser system, we have constructed the femtosecond laser irradiation platform for creating the quantum sensing device, such as NV centers. The femtosecond laser pulse is focused on a sample surface by an objective lens and laser pulse intensity is controlled by attenuators. By use of this irradiation apparatus, we have irradiated diamond samples to create NV centers. We could confirm several graphitization spots, but the signal intensity from NV center did not exist. To use the irradiation platform for creating NV centers in diamond, it needs some improvement, more increasing the repetition rate of irradiation laser and/or impurity nitrogen density in diamond sample.
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.
Emerging quantum technologies based on the nitrogen-vacancy (NV) centre in diamond require carefully engineered material with controlled defect density, optimised NV formation processes, and minimal crystal strain. The choice of NV generation technique plays a crucial role in determining the quality and performance of these centres. In this work, we investigate NV centre formation in nitrogen-doped diamond using femtosecond (fs) laser processing. We systematically examine the effect of laser pulse energy on NV production and quality using photoluminescence and optically detected magnetic resonance measurements. We also probe the role of pre-existing lattice defects formed by electron irradiation and consider defect evolution over extended dwell times. Finally, we are able to identify a regime where the main action of the fs-laser is to diffuse rather than create vacancies. This local annealing capability expands the toolkit for tailored NV production and presents opportunities for fine tuning defect populations.
Among quantum sensors, the single nitrogen-vacancy (NV) defect in diamond has the highest sensitivity-to-size factor. For instance, a single-NV spin when used as a magnetometer could achieve sensitivities of the order of nT/Hz, while the dimensions of the sensor are merely atomic in size. The sensitivity is limited only by the photon shot noise. One method to boost the magnetometer sensitivity to pico-tesla scales is to use many NV defect centers as an ensemble sensor [Phys. Rev. X5, 041001 (2015)PRXHAE2160-330810.1103/PhysRevX.5.041001]. However, during the absorption-emission (fluorescence) optical cycles, the NV centers transfer a portion of the irradiation laser energy into phonons and heat the diamond matrix. This results in unintended fluorescence decrease, spin resonance lines shifts, and fluctuations. Hence, the advantages gained by packing a high density of NV centers are significantly reduced. Here we investigate the heat generation of ensemble NV centers in micrometer-sized diamond under 532 nm laser irradiation and its effects pertaining to sensing applications. These investigations help us to find strategies that mitigate the detrimental effects of heating and yet permits the use of ensemble NV defects for improved metrology applications.
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.
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.