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Growth of thick CVD diamond films containing aligned nitrogen-vacancy centers for high-sensitivity quantum sensors

赳行 辻, Takeyuki Tsuji, 孝之 岩崎, Takayuki Iwasaki, 睦子 波多野, Mutsuko Hatano

Published Nov 1, 2022• 0 citations
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Here, we report the fabrication and characterization of single crystal diamond films on a two-inch wafer-scale containing three-dimensional layered structures of negatively charged nitrogen-vacancy color centers (NV−^{-}−). The (100)-oriented layered diamond films were grown by chemical vapor deposition (CVD) to create spatially separated regions of enhanced emission associated with NV−^{-}− centers. Such localized emission enhancement as well as 2D and 3D arrays of spins could enable close-packed architectures for emerging quantum devices, such as data processors, memory cells, and magnetic sensors. A cyclic sequence of CVD growth and oxygen-plasma etching is employed, resulting in the in-situ formation of layered inverted pyramidal structures with flat $\{111111111\}$ sidewalls. These pits are subsequently overgrown by nitrogen-doped diamond to achieve NV−^{-}−-rich facets with a uniform N-V bond arrangement and improved nitrogen incorporation efficiency.
We report the formation of perfectly aligned, high-density, shallow nitrogen vacancy (NV) centers on the (111) surface of a diamond. The study involved step-flow growth with a high flux of nitrogen during chemical vapor deposition (CVD) growth, which resulted in the formation of a highly concentrated (>1019 cm−3) nitrogen layer approximately 10 nm away from the substrate surface. Photon counts obtained from the NV centers indicated the presence of 6.1 × 1015–3.1 × 1016 cm−3 NV centers, which suggested the formation of an ensemble of NV centers. The optically detected magnetic resonance (ODMR) spectrum confirmed perfect alignment (more than 99%) for all the samples fabricated by step-flow growth via CVD. Perfectly aligned shallow ensemble NV centers indicated a high Rabi contrast of approximately 30% which is comparable to the values reported for a single NV center. Nanoscale nuclear magnetic resonance demonstrated surface-sensitive nuclear spin detection and provided a confirmation of the NV centers' depth. Single NV center approximation indicated that the depth of the NV centers was approximately 9–10.7 nm from the surface with error of less than ±0.8 nm. Thus, a route for material control of shallow NV centers has been developed by step-flow growth using a CVD system. Our finding pioneers on the atomic level control of NV center alignment for large area quantum magnetometry.