We report a systematic investigation on the spectral splitting of negatively charged, nitrogen-vacancy (NV − ) photoluminescent emission in single-crystal diamond induced by strain engineering. The stress fields arise from MeV ion-induced conversion of diamond to amorphous and graphitic material in regions proximal to the centers of interest. In low-nitrogen sectors of a high-pressure-high-temperature diamond, clearly distinguishable spectral components in the NV − emission develop over a range of ∼4.8 THz corresponding to distinct alignment of sub-ensembles which were mapped with micron spatial resolution. This method provides opportunities for the creation and selection of aligned NV − centers for ensemble quantum information protocols. Gesellschaft large optical dipoles and, in the case of the negatively charged nitrogen-vacancy (NV − ) center, long-lived ground-state coherence [3].Although much of the interest in NV − -based QIP is centered on room-temperature processes and isolated centers, there is also considerable interest in applying ensemble QIP protocols to the optical transition of inhomogeneously broadened NV − centers. Indeed the dipole moment and transition frequency for NV − are comparable to that of rubidium, meaning that translation of protocols developed for vapor cells is natural. Protocols using ensembles were initially considered for the first NV − quantum computing [4,5] and optical quantum non-demolition experiments [6]. There have been observations of long-lived ground-state coherence [7], coherent population trapping [8], magnetometry [9] and magnetic coupling between NV − ensembles and superconducting circuits [10,11].Despite the interest in ensemble processing with NV − , there are major challenges to be overcome, which place NV − at a disadvantage when compared with atomic vapors. One of the largest problems is the inhomogeneous linewidth and the nature of this inhomogeneity. The inhomogeneous linewidth of the optical transitions in NV − typically varies with strain [12], implantation strategy [13,14] and electric field [15], leaving the job of controlling the linewidth as a major goal of NV − engineering. Coupled to this problem is that at room temperature, the linewidth appears to be dominated by spectral diffusion, although exceptional emitters with almost lifetime-limited emission can be discovered [16][17][18][19][20], and there are no reports of ensembles of purely homogeneously broadened NV − centers.Here we show a new approach to spectrally separating aligned subensembles of NV − . By engineering permanent strain fields into the diamond lattice through ion implantation, we demonstrate that it is possible to resolve the orientationally inequivalent NV − subensembles based upon their spectral properties. These results reveal new opportunities for the use of aligned, inhomogeneously broadened ensembles of NV − centers for QIP that is distinct from more traditional methods of applying external uniaxial strain to a lattice.In the study of defect-related optical transitions in cryst...