We report the observation of an unusual behavior of highly extended 5d electrons in Y2Ir2O7 belonging to pyrochlore family of great current interest using high resolution photoemission spectroscopy. The experimental bulk spectra reveal an intense low
er Hubbard band in addition to weak intensities in the vicinity of the Fermi level, e_F. This provides a direct evidence for strong electron correlation among the 5d electrons, despite their highly extended nature. The high resolution spectrum at room temperature exhibits a pseudogap at e_F and |e - e_F|^2 dependence demonstrating the importance of electron correlation in this system. Remarkably, in the magnetically ordered phase (T < 150 K), the spectral lineshape evolves to a |e - e_F|^1.5 dependence emphasizing the dominant role of electron-magnon coupling.
We investigate the spin state of LaCoO3 using state-of-the-art photoemission spectroscopy and ab initio band structure calculations. The GGA+U calculations provide a good description of the ground state for the experimentally estimated value of elect
ron correlation strength, U. In addition to the correlation effect, spin-orbit interaction is observed to play a significant role in the case of intermediate spin and high spin configurations. The comparison of the calculated Co 3d and O 2p partial density of states with the experimental valence band spectra indicates that at room temperature, Co has dominant intermediate spin state configuration and that the high spin configuration may not be significant at this temperature. The lineshape of the La 5p and O 2s core level spectra could be reproduced well within these ab initio calculations.
