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Mechanism and control of the metal-to-insulator transition in rocksalt tantalum nitride

We identify the previously unknown mechanism whereby rocksalt Ta x N can be continuously tuned from conducting to insulating through changes in stoichiometry. Experimental measurements on thin films, combined with electronic structure calculations on a host of native defects, show that the tunability arises from changes in the free electron concentration as a result of localization at Ta vacancies (V T a ). The observed enhanced resistivity, transition from electron to hole conduction at x∼0.6, and diminished mid-IR reflectance are consistent with the dominance of the V T a defect in nitrogen-rich material.