Abstract With their optical addressability of individual spins and long coherence time, nitrogen-vacancy (NV) centers in diamond are often called “atom-like solid spin-defects”. As observed with trapped atomic ions, quantum interference mediated by indistinguishable photons was demonstrated between remote NV centers. In high sensitivity DC magnetometry at room temperature, NV ensembles are potentially rivaling with alkali-atom vapor cells. However, local strain induces center-to-center variation of both optical and spin transitions of NV centers. Therefore, advanced engineering of diamond growth toward crystalline perfection is demanded. Here, we report on the synthesis of high-quality HPHT (high-pressure, high-temperature) crystals, demonstrating a small inhomogeneous broadening of the spin transitions, of T 2 * = 1.28 μs, approaching the limit for crystals with natural 13 C abundance, that we determine as T 2 * = 1.48 μs. The contribution from strain and local charges to the inhomogeneous broadening is lowered to ~17 kHz full width at half maximum for NV ensemble within a > 10 mm 3 volume. Looking at optical transitions in low nitrogen crystals, we examine the variation of zero-phonon-line optical transition frequencies at low temperatures, showing a strain contribution below 2 GHz for a large fraction of single NV centers.
Abstract With their optical addressability of individual spins and long coherence time, nitrogen-vacancy (NV) centers in diamond are often called “atom-like solid spin-defects”. As observed with trapped atomic ions, quantum interference mediated by indistinguishable photons was demonstrated between remote NV centers. In high sensitivity DC magnetometry at room temperature, NV ensembles are potentially rivaling with alkali-atom vapor cells. However, local strain induces center-to-center variation of both optical and spin transitions of NV centers. Therefore, advanced engineering of diamond growth toward crystalline perfection is demanded. Here, we report on the synthesis of high-quality HPHT (high-pressure, high-temperature) crystals, demonstrating a small inhomogeneous broadening of the spin transitions, of T 2 * = 1.28 μs, approaching the limit for crystals with natural 13 C abundance, that we determine as T 2 * = 1.48 μs. The contribution from strain and local charges to the inhomogeneous broadening is lowered to ~17 kHz full width at half maximum for NV ensemble within a > 10 mm 3 volume. Looking at optical transitions in low nitrogen crystals, we examine the variation of zero-phonon-line optical transition frequencies at low temperatures, showing a strain contribution below 2 GHz for a large fraction of single NV centers.
Negatively charged nitrogen vacancy (NV−) centres in diamond crystals are promising colour centres for high-sensitivity quantum sensors. A long dephasing time (T2* > 10 μs) is essential for achieving increased sensitivity and higher uniformity of T2* in millimetre-scale diamond is strongly desired for femto-tesla weak magnetic field detection. High uniformity of T2* for NV− centres is achieved herein. The median value of T2*, <T2*>, in the 12C-enriched high-pressure, high-temperature (HPHT) grown diamond with a nitrogen concentration of 1.3 ± 0.4 ppm is 4.5 μs. The variance of T2* is only 10% over a millimetre-scale region (1.1 × 1.1 mm2) within the 0.4 mm thick {111} growth sector. <T2*> is ~2/3 times the value limited by the dipole-dipole interaction from the electron-spin bath of nitrogen impurities, suggesting that the residual strain gradient in the HPHT diamond crystal partially limits T2*. Reducing the strain gradient in diamond crystals provide a pathway to achievement of high sensitivity magnetometry using NV quantum sensing. Negatively charged nitrogen vacancy centres in diamond crystals are promising for achieving high-sensitivity quantum sensors. Here, a long dephasing time with high uniformity is achieved in a millimetre-scale area along the {111} plane using 12C enriched high-pressure high-temperature diamond crystals.
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 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.
Nitrogen-vacancy (NV) centers in diamond with coherent optical transitions are a promising candidate for quantum science and technology protocols. A widely used strategy for their creation is nitrogen-ion implantation and high-temperature annealing. The data presented in this work show that while low-strain, narrow-optical-linewidth NV centers are formed from naturally occurring 14N atoms, NV centers formed from the implanted 15N atoms show broadened optical transitions and experience higher strain. These results have immediate implications for the positioning accuracy of current NV center creation protocols.
Silicon-vacancy (SiV) color centers in diamond offer a promising system for quantum information applications owing to their intense narrowband emission and optically detectable spin states. Here, the fluorescent properties of ensembles and single SiV centers in diamonds obtained by high-pressure high-temperature synthesis from adamantane (below referred to as adamantane diamonds) are investigated at liquid-helium temperatures. Ensembles of SiV centers (~10 3 ) are studied in large diamond crystals (1–2 µm in size). Despite the large number of excited centers, the fine structure of the zero-phonon line, corresponding to four allowed optical transitions between the ground- and excited-state doublets of the SiV center, can be observed in the fluorescence spectra of these crystals. The width of individual lines is in the range of 60–80 GHz, which is explained by their inhomogeneous broadening. Single SiV centers are studied in diamond crystallites with sizes of about 200 nm. The width of the narrowest transition lines observed in the fluorescence spectra of single SiV centers under resonant excitation is almost three orders of magnitude smaller than linewidths in the spectra of SiV ensembles and is as small as 94 MHz; i.e., these lines are so narrow that their width is determined by the lifetime of the upper state of the transition. Therefore, adamantane nanodiamond features the narrowest emission line width of a single SiV center at cryogenic temperatures among other types of SiV-con-taining nanodiamonds of similar sizes obtained by the high-pressure high-temperature and chemical vapor deposition techniques.
The negatively charged nitrogen-vacancy (NV) center in diamond is among the most promising solid-state systems implementations of a quantum bit. However, integration of the NV center into any efficient photonic environment requires microstructuring the diamond at below-micrometer scale. Preserving the low NV zero-phonon line inhomogeneous broadening during this process is a major challenge with standard NV creation methods. This issue severely limits practical applications of NV centers. Initial studies on pulsed-laser assisted creation of NVs yielded promising results by creating NVs with low inhomogeneous broadening at desired spatial locations in diamond [1]. Crucially, the lattice damage resulting from implantation of energetic ions was avoided. However, the method relied on a narrow window of parameters for successful writing. We widen this window by using a solid immersion lens (SIL), which facilitates laser writing over a broad range of pulse energies and allows for vacancy formation close to a diamond surface without inducing surface graphitization. We operate in the previously unexplored regime where lattice vacancies are created following tunneling breakdown rather than multiphoton ionization [2]. We present NV arrays that have been created between 1 and 40 µm from a diamond surface, all presenting optical linewidth distributions with means as low as 61.0±22.8 MHz [2], including spectral diffusion induced by off-resonant repump for charge stabilization. This emphasizes the exceptionally low charge-noise environment of laser-written NVs. Such high-quality NV centers are excellent candidates for practical applications employing two-photon quantum interference with separate NV centers. Finally, we propose a model for disentangling power broadening from inhomogeneous broadening in the NV zero-phonon line optical linewidth [2]. [1] Y.-C. Chen, P. S. Salter, S. Knauer, … and J. M. Smith, Nat. Photonics 11, 77 (2017). [2] V. Yurgens, J.A Zuber, S. Flågan, M. De Luca, B.J. Shields, I. Zardo, P. Maletinsky, R.J. Warburton, and T. Jakubczyk, ACS Photonics 8, 1726–1734 (2021)