Harnessing Diamond Surface Features for Dense and Aligned NV Ensembles

Controlling nitrogen doping in diamond is key to advancing nitrogen-vacancy (NV) center devices. We harness the hillock, a typically undesirable surface feature, to incorporate high densities of grown-in, aligned NV centers on a (001)-oriented substrate. Enhanced cathodoluminescence at hillock sidewalls is correlated via nanoSIMS to up to 1000× greater nitrogen incorporation compared to the planar film. We find that these hillocks are associated with stacking faults and edge-type dislocations, consistent with an origin in surface preparation rather than substrate screw dislocations. Yet, the growth is orderly enough that each of the four hillock sidewalls hosts a distinct NV orientation. A 1.7-2% grown-in NV/substitutional nitrogen (P1) ratio, 4× higher than typical (001)-oriented growth, is measured via NV decoherence analysis. By revealing that spontaneously formed hillocks act as natural laboratories for dense, aligned NV formation, this work motivates systematic investigation of facet-dependent nitrogen incorporation and preferential NV alignment in (001) diamond.