Mott-Hubbard insulator-metal transition in the VO2 thin film: A combined XAS and resonant PES study

We have analyzed spectral weight changes in the conduction and the valence band across insulator to metal transition (IMT) in the VO2 thin film using X-ray absorption spectroscopy (XAS) and resonant photoemission spectroscopy (PES). Through temperature dependent XAS and resonant PES measurements we unveil that spectral changes in the d$_{\|}$ states (V 3$\it{d_{x^2-y^2}}$ orbitals) are directly associated with temperature dependent electrical conductivity. Due to presence of the strong electron-electron correlations among the d$_{\|}$ states, across IMT, these states are found to exhibit significant intensity variation compared to insignificant changes in the $π^{\ast}$ and the $σ^{\ast}$ states (which are O 2$\it{p}$ hybridized V 3$\it{d}$ $e_g^π$ and $e_g^σ$ states) in the conduction band. Experimentally obtained values of the correlation parameter (U$_{dd}$ $\sim$ 5.1 eV, intra-atomic V 3$\it{d}$ correlations) and crystal field splitting (10 Dq $\sim$ 2.5 eV) values are used to simulate the V $\it{L_{2,3}}$ edge XAS spectra and an agreement between simulated and experimental spectra also manifests strong correlations. These results unravel that the IMT observed in the VO2 thin film is the Mott-Hubbard insulator-metal transition.