Solid-state spin defects are a promising platform for quantum networks. A key requirement is to combine long ground-state spin-coherence times with a coherent optical transition for spin-photon entanglement. Here, we investigate the spin and optical coherence of single nitrogen-vacancy (NV) centres in (111)-grown isotopically engineered diamond. Our diamond-growth process yields a precisely controlled
13C concentration and low-ppb nitrogen concentrations. Combined with the mitigation of 50 Hz noise using a real-time feedforward scheme and tailored decoupling sequences, this enables record defect-electron-spin coherence times of
T2=6.8(1) ms for a Hahn echo and of
T2DD=11.2(8) s under dynamical decoupling. In addition, we observe coherent optical transitions with a near-lifetime-limited homogeneous linewidth of 16.9(4) MHz and characterize the spectral diffusion dynamics. These results provide new avenues to investigate the incorporation of impurities in diamond and new opportunities for improved spin-qubit control for quantum networks and other quantum technologies.
Since nitrogen-vacancy (NV) centers in diamond have emerged as crucial quantum sensors in physics and biology, the massive preparation of high-quality and high-concentration shallow NV center samples has become urgent and demanding. As NV centers approach the surface and their concentration increases, charge state instability can degrade coherence and introduce additional noise. This problem is further complicated in high-pressure and high-temperature (HPHT) diamonds due to the presence of unclear impurities and inhomogeneous strain. Through optically detected magnetic resonance testing on various implanted samples, we analyzed the spin and charge state properties of shallow NV center ensembles. Our results reveal that the doping dose significantly influences the quantity of NV−, charge, and charge stability. Our findings indicate that over-implanting nitrogen as electron donors before starting graphitization helps stabilize the charge environment of the shallow NV center ensembles. By controlling the nitrogen ion implantation dose, we optimized charge state stability under photoionization and prepared high-quality NV center ensemble samples in HPHT diamonds at the optimal implantation dose range of 2×1013–8×1013 ions/cm2. This method, which relies solely on nitrogen ion implantation and annealing on HPHT diamond, significantly reduces the cost of sensor samples, greatly benefiting the promotion of quantum sensing.
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.
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.
A nitrogen vacancy (NV) center in diamond is known as a solid-state spin quantum bit (qubit) at room temperature. The fabrication of scalable quantum registers based on NV centers is a long-standing issue. In 2005, spin-spin interaction between NV-N pairs, which were fabricated by N2 ion implantation, was reported. An entanglement between two electron-spin qubits becomes an excellent quantum information processing component, as accomplished by an NV-NV pair with a nanometer-scale distance in 2010 and 2013. More recently,strongly dipolar coupled NV-NV pairs were realized by 14N 30 keV implantationvia nanoholes in PMMA resist mask. The creation yields of NV-NV pairs dramatically improved, and the nanohole implantation had been thought to be the most promising technique to integrate NV centers. However, the problem of the technique is the finite size of nanoholes. The distribution of nitrogen atoms is determined by both ion straggling and nanohole diameter. The scaling of NV centers is stagnant up to two for several years. To overcome the barrier of triple NV centers, our previous research gave a ground-breaking idea of a highly populated NV center complex by introducing a molecular ion implantation technique in 2019. Since the molecular ion is regarded as an idea point source, the distribution of nitrogen atoms is determined by only ion straggling. Therefore, our proposed method is more effective than other implantation techniques including nanohole implantation. Instead of a pure nitrogen cluster which is commonly unstable, the stable organic molecular ions (adenine; C5N5H5) were utilized as the ion source. We successfully implanted C5N4Hn ions into single crystalline diamonds. Three NV centers were integrated, and the dipolar interactions among them were successfully observed. In 2022, we succeeded in creating more than 5 NV centers by phthalocyanine (C32H18N8) ion implantation. The next challenge is the implantation of isotopically enriched molecular ions. The isotopically enriched ion contains 13C and 15N. The implantation of isotopically enriched molecular ions is able to create 15NV-13C hybrid quantum registers. In this presentation, we will show the development of the isotopically enriched molecular ion beam and the characterization of created NV centers by laboratory-built confocal microscopy (CFM) and optically detected magnetic resonance (ODMR).