Structure électronique et magnétique des oxydes de métaux de transition : le cas de Fe3O4

Magnetite (Fe3O4) is a promising candidate for application in spintronic devices. This ferrimagnet with a high Curie temperature has been theoretically predicted to be a half-metal with a conductive minority-spin (↓) channel and a semiconductive majority-spin (↑) channel, resulting in 100 % spin polarization at the Fermi level. But up to now, any clear experimental evidence is lacking. This thesis presents spin- and angle-resolved photoemission studies on the magnetic and electronic structure of Fe3O4 (001) epitaxially grown on MgO (001). A band structure calculation using generalized gradient approximation plus U (GGA+U) to the density functional theory (DFT) is proposed to explain the experimental results. Although the PES intensity at Fermi level is very low because of the role played by polarons, a dispersion of the Fe 3d-t2g states is observed. The overall behaviour of these bands is in good agreement with the calculation of ground state electronic structure. In order to simulate the spectra, we used the free electron approximation for the final states, ignoring the matrix elements. Calculated ground state data are convoluted by Lorentzian and Gaussian functions to account for the lifetime and electron-phonon coupling effects, respectively. By integrating the spectral intensity over an energy interval of 100meV at Fermi level, we obtained the first experimental evidence of the Fermi surface plot. Determination of electron spin polarization is an ultimate test of both the band calculations and our model of Fe3O4 photoemission spectra. In our spin-resolved photoemission experiments 4.65 and 6.20 eV photons were used. The same sample was used as for spin-integrated ARPES, requiring its transfer through air to another chamber. It was not subject to any cleaning prior to the SRPES measurements that lead to a reduction of the spin polarization as a consequence of the presence of a dead layer on the surface. Nevertheless the spin polarization close to EF reaches - 50% and -72% for 6.20 and 4.65 eV photons respectively. We conclude that Fe3O4 can be described within a band model and in particular that it is half-metallic. We also used femtosecond laser pulses in pump-probe experiments to investigate ultrafast dynamics on atomic scale. Our results show that the lifetime of excited electrons in Fe3O4 is much longer than in an “ordinary” metal. From the spin analysis of excited electrons, we deduce that the demagnetization does not occur in the femtosecond range, which is compatible with half-metallic properties of magnetite.