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金刚石氮-空位（NV）色心在室温下稳定性好，电子自旋相干时间长，能被激光和微波操控，是量子探测领域最具潜力的结构。本研究采用微波等离子化学气相沉积法（MPCVD）制备具有较高氮含量的金刚石单晶，以构建高浓度NV色心。通过在前驱体气体中掺杂不同含量的氮原子，解决了高氮条件下长时间生长金刚石单晶出现的诸多问题，制备氮含量约为0.205ppm、5ppm、8ppm、11ppm、15ppm、36ppm和54ppm的高氮金刚石单晶。初步确定了前驱体气体中氮含量与进入到金刚石单晶晶格中氮含量的关系平均约为11，氮原子在金刚石单晶中主要以聚集态氮和单个替位N+形式存在。对高氮金刚石单晶进行电子辐照，显著提升了金刚石NV色心浓度，并对辐照后NV色心材料的磁探测性能进行验证。Diamond nitrogen vacancy (NV) color centers have good stability at room temperature, long electron spin coherence time, and can be manipulated by lasers and microwaves, making them the most promising structure in the field of quantum detection. Within a certain range, the higher the concentration of NV color centers, the higher the sensitivity of detecting physical quantities. Therefore, it is necessary to dope sufficient nitrogen atoms into diamond single crystals to form high concentration of NV color centers. In this study, diamond single crystals with different nitrogen content were prepared by microwave plasma chemical vapor deposition (MPCVD) to construct high concentrations of NV color centers. By doping different amounts of nitrogen atoms into the precursor gas, many problems encountered during long-time growth of diamond single crystals under high nitrogen conditions were solved. Diamond single crystals with nitrogen contents of approximately 0.205 ppm, 5 ppm, 8 ppm, 11 ppm, 15 ppm, 36 ppm, and 54 ppm were prepared. As the nitrogen content increased, the width of the step flow on the surface of the diamond single crystal gradually widened, eventually the step flow gradually disappeared and the surface became smooth. Under the experimental conditions of this study, it was preliminarily determined that the average ratio of the nitrogen content in the precursor gas to the nitrogen atoms content introduced into the diamond single crystal lattice was about 11. Fourier transform infrared spectroscopy shows that as the nitrogen content inside the CVD diamond single crystal increases, the density of vacancy defects also increases. Therefore, the color of CVD high nitrogen diamond single crystals ranges from light brown to brownish black. Compared with HPHT diamond single crystals, the intensity of absorption peak at 1130cm-1 is weaker, absorption peak at 1280cm-1 was not shown. Three obvious nitrogen related absorption peaks at 1371cm-1, 1353cm-1, and 1332cm-1 of CVD diamond single crystal were displayed. Nitrogen atoms mainly exist in the form of aggregated nitrogen and single substitutional N+ in diamond single crystals, rather than in the form of C-defect. The PL spectra results showed that defects such as vacancies inside the diamond single crystal with nitrogen content of 54 ppm were significantly increased after electron irradiation, leading to a remarkable increase in the concentration of NV color centers. The magnetic detection performance of the NV color center material after irradiation was verified, the fluorescence intensity was uniformly distributed in the sample surface. The diamond single crystal with nitrogen content of 54 ppm had good microwave spin manipulation, its longitudinal relaxation time was about 3.37 ms.
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Keywords:
- Diamond single crystal /
- High content of Nitrogen /
- NV color center /
- FTIR /
- Magnetic detection
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