Cooperative Effects of Strain and Electron Correlation in Epitaxial VO2 and NbO2

Abstract: We investigate the electronic structure of the epitaxial VO$2$ films in the rutile phase using the density functional theory combined with the slave spin method (DFT+SS). In DFT-SS, the multiorbital Hubbard interactions are added to a DFT-fit tight-binding model, and we employ the slave-spin method to treat the electron correlation. We find that while stretching the system along the rutile $c$-axis results in a band structure favoring an anisotropic orbital fillings, the electron correlation favors an equal electron filling among $t{2g}$ orbitals. These two distinct effects cooperatively induce interesting orbital-dependent redistributions of the electron occupations and the spectral weights, which pushes the strained VO$_2$ toward an orbital selective Mott transition (OSMT). The simulated single-particle spectral functions are directly compared to V L-edge resonant X-ray photoemission spectroscopy of epitaxial 10 nm VO$_2$/TiO$_2$ (001) and (100) strain orientations. Excellent agreement is observed between the simulations and experimental data regarding the strain-induced evolution of the lower Hubbard band. Simulations of rutile NbO$_2$ under similar strain conditions as VO$_2$ are performed, and we predict that OSMT will not occur in rutile NbO$_2$. Our results indicates that the electron correlation in VO$_2$ is important and can be modulated even in the rutile phase before the Peierls instability sets in.