Synthetic diamond production is key to the development of quantum metrology and quantum information applications of diamond. The major quantum sensor and qubit candidate in diamond is the nitrogen-vacancy (NV) color center. This lattice defect comes in four different crystallographic orientations leading to an intrinsic inhomogeneity among NV centers that is undesirable in some applications. Here, we report a microwave plasma-assisted chemical vapor decomposition (MPCVD) diamond growth technique on (111)-oriented substrates that yields perfect alignment ($94pm2%$) of as-grown NV centers along a single crystallographic direction. In addition, clear evidence is found that the majority ($74pm4%$) of the aligned NV centers were formed by the nitrogen being first included in the (111) growth surface and then followed by the formation of a neighboring vacancy on top. The achieved homogeneity of the grown NV centers will tremendously benefit quantum information and metrology applications.
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