Strain‐Mediated High Conductivity in Ultrathin Antiferromagnetic Metallic Nitrides

Abstract Strain engineering provides the ability to control the ground states and associated phase transition in epitaxial films. However, the systematic study of the intrinsic character and strain dependency in transition‐metal nitrides remains challenging due to the difficulty in fabricating stoichiometric and high‐quality films. Here the observation of an electronic state transition in highly crystalline antiferromagnetic CrN films with strain and reduced dimensionality is reported. By shrinking the film thickness to a critical value of ≈ 30 unit cells, a profound conductivity reduction accompanied by unexpected volume expansion is observed in CrN films. The electrical conductivity is observed surprisingly when the CrN layer is as thin as a single unit cell thick, which is far below the critical thickness of most metallic films. It is found that the metallicity of an ultrathin CrN film recovers from insulating behavior upon the removal of the as‐grown strain by the fabrication of freestanding nitride films. Both first‐principles calculations and linear dichroism measurements reveal that the strain‐mediated orbital splitting effectively customizes the relatively small bandgap at the Fermi level, leading to an exotic phase transition in CrN. The ability to achieve highly conductive nitride ultrathin films by harnessing strain‐control over competing phases can be used for utilizing their exceptional characteristics.