Electronic structure of CrO2 probed by NMR and DFT

The electronic structure of ferromagnetic half-metal CrO2 was studied by means of 53Cr nuclear magnetic resonance (NMR) spectroscopy and density functional theory (DFT). The measured NMR spectrum consists of three distinct spectral lines and is interpreted as a triplet arising due to electric quadrupole interaction. The observed NMR parameters agree well with those obtained from electronic structure calculations, corresponding to the presence of Cr4+ with fully occupied localized dxy singlet and partially occupied degenerated dxz and dyz states, as required by the ferromagnetic double exchange mechanism. With high accuracy, the orbital occupations and valence states of all Cr atoms within the CrO2 structure are found to be uniform.