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arXiv:2409.17442 · Physical Review Applied

Optically coherent nitrogen-vacancy centers in high-pressure-high-temperature-treated diamonds

Yuan-Han Tang, Xiaoran Zhang, Kang‐Yuan Liu, Fan Xia, Huijie Zheng, Xiaobing Liu, Xinyu Pan, Heng Fan, Gang‐Qin Liu

Published May 30, 2025• 4 citations
arXivHTMLPDF

Abstract

Nitrogen-vacancy (N-$V$) centers in diamond are widely used in quantum information science, but existing methods to fabricate N-$V$ centers rely on damaging the diamond lattice, and usually lead to poor optical coherence. The authors propose a nondestructive method, where high-purity diamonds are annealed under high pressure and high temperature, to generate N-$V$ centers with excellent optical, spin, and charge properties. These results provide new insights into the diffusion dynamics of defects under extreme conditions, and indicate that even the ultrapure diamond contains enough nitrogen and vacancies to form N-$V$ centers.

DOI
10.1103/physrevapplied.23.054092

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Nitrogen-vacancy (N-VVV) centers in diamond are widely used in quantum information science, but existing methods to fabricate N-VVV centers rely on damaging the diamond lattice, and usually lead to poor optical coherence. The authors propose a nondestructive method, where high-purity diamonds are annealed under high pressure and high temperature, to generate N-VVV centers with excellent optical, spin, and charge properties. These results provide new insights into the diffusion dynamics of defects under extreme conditions, and indicate that even the ultrapure diamond contains enough nitrogen and vacancies to form N-VVV centers.
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.
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.
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.
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 14{}^{14}14N atoms, NV centers formed from the implanted 15{}^{15}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.
Single color centers in solid have emerged as promising physical platforms for quantum information science. Creating these centers with excellent quantum properties is a key foundation for further technological developments. In particular, the microscopic understanding of the spin-bath environments is the key to engineer color centers for quantum control. In this work, we propose and demonstrate a distinct high-temperature annealing (HTA) approach for creating high-quality nitrogen vacancy (N-V) centers in implantation-free diamonds. Simultaneously using the created N-V centers as probes for their local environment we verify that no damage is microscopically induced by the HTA. Nearly all single N-V centers created in ultralow-nitrogen-concentration membranes possess stable and Fourier-transform-limited optical spectra. Furthermore, HTA strongly reduces noise sources naturally grown in ensemble samples, and leads to more than threefold improvements of decoherence time and sensitivity. We also verify that the vacancy activation and defect reformation, especially H3 and P1 centers, can explain the reconfiguration between spin baths and color centers. This distinct approach will become a powerful tool in vacancy-based quantum technology.