Nitrogen-vacancy (NV) centers in diamond have attracted significant interest because of their excellent spin and optical characteristics for quantum information and metrology. To exploit these characteristics, precise control of the orientation of the NV axis in the lattice is essential. Here we show that the orientation of more than 99% of the NV centers can be aligned along the [111] axis by chemical vapor deposition homoepitaxial growth on (111) substrates. We also discuss the alignment mechanisms. Our result enables a fourfold improvement in the magnetic field sensitivity and opens new avenues to the optimum design of NV center devices.
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