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.
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.
ABSTRACT With unique optical and spin properties, the negatively charged nitrogen‐vacancy (NV − ) center in diamond has become a leading physical platform for quantum information processing. Fabrication of NV centers involves three steps: introducing nitrogen atoms, creating lattice vacancies, and combining these two types of defects. The final step is typically achieved by high‐temperature annealing, as vacancy migration in diamond is thermally activated above 600°C. Compared to low‐pressure high‐temperature (LPHT) annealing, high‐pressure and high‐temperature (HPHT) treatment allows for much higher annealing temperatures and longer durations, providing new opportunities to optimize key metrics of NV centers. This short review summarizes recent experimental progress in this direction. Dense NV centers with good spin coherence and single NV centers with excellent optical properties have been produced through HPHT growth and post‐treatment of single‐crystal diamonds. In addition, structural imaging, optical characterization, and DFT calculations provide further insights into the dynamics of defect migration under high‐temperature annealing. These results offer new perspectives on the fabrication of color centers in diamond and other wide‐gap semiconductor materials, including silicon carbide and hexagonal boron nitride, for advanced quantum applications.
Silicon has turned from a niche laboratory-scale material into the backbone of modern electronics. Diamond functionalized with color centers could follow a similar path and grow from proof-of-concepts experiments to application-oriented quantum technologies. Quantum sensing, communication, and information processing with color centers has been proven to work in scientific experiments and enhanced sensitivities as well as novel functionalities have been reported. While the first generation of diamond quantum devices relied on color centers formed uncontrolled in natural diamond with a high statistical variation in composition and crystallinity, the situation has changed nowadays. With the emergence of high purity monocrystals and the option for isotopic purification of the carbon matrix, technological progress in materials science on the atomic-scale enabled tailoring the spin properties in diamond. But, since many color centers typically require vacancies to combine with impurities in the carbon lattice via diffusion, the generation of color centers underlies a statistical process providing only little control on the center's final position in the crystal lattice. The negatively charged nitrogen-vacancy (NV
−) center is the most studied optically active defect in diamond and exhibits remarkable spin properties and sensing capabilities, even on the nanoscale and at room temperature. The spin properties of NV
− centers close to the surface (1\,nm - 30\,nm) have been thoroughly studied and the deeper the spins are located in diamond the less decoherence from surface defects is observed. Creating NV
− centers at the surface by nitrogen ion implantation and burying them beneath a thin diamond layer via chemical vapor deposition (CVD) of diamond is reported to enhance the coherence times significantly. By separating the color center generation from controlling the resulting depth by an additional diamond layer, narrow depth profiles can be achieved by reducing the ion energy during implantation. Although the coherence properties improve, many of the implanted NV
− center are reported to vanish in the hydrogen-rich plasma of growth CVD chambers. The mechanism responsible for the instability of NV
− centers towards the plasma remains unclear, though. One hypothesis is the formation of nitrogen-vacancy-hydrogen centers from diffusing hydrogen and implanted NV
− centers but is has not been proven, yet. Here, we demonstrate the fabrication of depth confined NV
− centers by combining low energy (1\,keV - 5\,keV) ion implantation and CVD overgrowth. By increasing the thickness of the overgrown layer (6\,nm - 100\,nm) the influence of surface noise is shown to decrease leading to bulk-like coherence properties of up to $450\,\upmu$s (Hahn-echo) and
T2∗ dephasing times around $20\,\upmu$s. Monitoring the NV
− density as a function of the overgrowth time, we analyze the kinetics of the passivation in case of implanting ion doses of 10
11 15N
+/cm
2 and 10
12 15N
+/cm
2. The passivation turns out to occur faster for lower doses offering insights into sub-surface hydrogen diffusion in diamond. Analyzing the spin bath before and after overgrowth reveals a drastic reduction in paramagnetic spins after the CVD process but no NVH
− is found around the surviving NV
− centers. Checking the chemical composition in overgrown implantation sites with secondary-ion-mass-specrometry (SIMS), however, confirms significant amounts of hydrogen in the
15N-implanted layers. Since the concentration found for hydrogen exceeds the one for nitrogen by far, we suggest that diffusing hydrogen interacts also with vacancies forming probably mostly diamagnetic defects. In the last part of this dissertation, NV
− centers are generated with sub-nanometer precision below a thin
13C-enriched layer for quantum simulation. For fabricating the spin architecture starting from a
12C base layer, we overgrow implanted nitrogen with a
13C layer and bury the spins beneath a 30\,nm-thick
12C capping layer. By measuring the coupling strength between the electron and nuclear spins, we deduce a NV
− placement accuracy reaching below one nanometer with respect to the
13C-layer. Regarding the spin properties of the electron spins, no reduction in
T2 is observed despite of the proximity to the dense
13C-bath. As a consequence, the overgrowth of NV
− centers is demonstrated as a bottom-up approach to produce buried spin architectures with sharp isotopic transitions and efficient
13C-NV
− coupling. Together with the potential for bulk-like coherence properties the synergy of implantation and overgrowth is a powerful tool to fabricate reproducible quantum systems with tailored properties and high depth confinement.
Abstract Single negatively charged nitrogen vacancy (NV−) centers in diamond have emerged as promising platforms for quantum information science, where long coherence times are essential for advancing quantum technologies. However, traditional fabrication methods often introduce lattice damage during the irradiation process used to create vacancies, significantly impairing the spin coherence properties of NV− centers. In this study, we systematically investigate high-pressure/high-temperature (HPHT) annealing as a non-destructive approach to generate high-coherence single NV− centers and elucidate the underlying mechanisms. Our results reveal that the distortion of the lattice field significantly influences the preferential formation of NV− centers at the interface of the 〈111〉-growth sector during diamond crystallization. Moreover, HPHT annealing effectively mobilizes nitrogen and vacancies, significantly promoting the formation of single NV− centers. This process also mitigates the influence of the distortion of the lattice field, resulting in a marked enhancement of coherence properties, with T 2 times reaching 578 μs. Notably, a naturally formed single NV− center in a low-stress region achieves an exceptional T 2 time of 721 μs, representing one of the highest values reported for diamonds with natural 13C abundance. Building on these insights, we have successfully achieved controlled, large-scale fabrication of high-coherence single NV− centers, providing essential guidance for future efforts to further enhance their coherence and establishing a robust foundation for their application in quantum technologies.
Abstract The high‐pressure and high‐temperature (HPHT) diamonds with well‐controlled defects and low stress offer an ideal host substrate for the fields of quantum information science; however, fabrication of quantum‐grade HPHT diamonds remains a pressing challenge. Here, a major advance in generating highly coherent nitrogen‐vacancy (NV) centers, a promising spin defect in diamonds, via tailored HPHT synthesis and postgrown annealing treatment is reported. The resulting well‐dispersed single NV− centers in type‐IIa diamonds exhibit long spin coherence times comparable to that of the reported chemical vapor deposition diamonds. Moreover, high‐density NV− ensembles in 〈100〉‐grown type‐Ib diamonds with superb zero‐phonon lines considerably sharper than those of native NV− centers in as‐grown diamonds, together with low splitting of resonances are produced. These findings demonstrate a superior synthesis and optimization protocol for creating high‐quality NV− centers avoiding lattice damage in diamond to meet the stringent requirements for a wide range of emerging quantum technologies.