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 1000x 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, 4x 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.