Determination of the orbital moment and crystal-field splitting in LaTiO3

Utilizing a sum rule in a spin-resolved photoelectron spectroscopic experiment with circularly polarized light, we show that the orbital moment in LaTiO3 is strongly reduced from its ionic value, both below and above the Ne el temperature. Using Ti L2,3 x-ray absorption spectroscopy as a local probe, we found that the crystal-field splitting in the t2g subshell is about 0.12-0.30 eV. This large splitting does not facilitate the formation of an orbital liquid.     

d-d excitations in manganites probed by resonant inelastic x-ray scattering

We report a study of electronic excitations in manganites exhibiting a range of ground states, using resonant inelastic x-ray scattering (RIXS) at the Mn K edge. Excitations with temperature dependent changes correlated with the magnetism were observed as high as 10 eV. By calculating Wannier functions, and finite-q response functions, we associate this dependence with intersite d-d excitations. The calculated dynamical structure factor is found to be similar to the RIXS spectra.     

Orbital nature of ferromagnetic magnons in manganites

Magnon excitation in a ferromagnetic state of Sm(0.55)Sr(0.45)MnO(3) located on the verge of the metal-insulator transition has been studied in terms of the neutron scattering experiment. The anomalous magnon dispersion with the zone-boundary softening is well described by the Heisenberg model with extended exchange coupling constants J(s). In particular the fourth neighbor coupling J(4) is as large as 0.6 times the nearest neighbor one J(1). Theoretical analysis based on the local density approximation + Hubbard U band calculation reveals that this one-dimensional exchange path is due to the (3z(2)-r(2))-type orbital correlation, in sharp contrast to previous proposals.     

Observation of a griffiths phase in paramagnetic La1-xSrxMnO3

We report on the discovery of a novel triangular phase regime in the system La1-xSrxMnO3 by means of electron spin resonance and magnetic susceptibility measurements. This phase is characterized by the coexistence of ferromagnetic entities within the globally paramagnetic phase far above the magnetic ordering temperature. The nature of this phase can be understood in terms of Griffiths singularities arising due to the presence of correlated quenched disorder in the orthorhombic phase.     

Soft x-ray resonant diffraction study of magnetic and orbital correlations in a manganite near half doping

We have utilized resonant x-ray diffraction at the Mn L(II,III) edges in order to directly compare magnetic and orbital correlations in Pr0.6Ca0.4MnO3. Comparing the widths of the magnetic and orbital diffraction peaks, we find that the magnetic correlation length exceeds that of the orbital order by nearly a factor of 2. Furthermore, we observe a large (approximately 3 eV) spectral weight shift between the magnetic and orbital resonant line shapes, which cannot be explained within the classic Goodenough picture of a charge-ordered ground state. To explain the shift, we calculate the orbital and magnetic resonant diffraction line shapes based on a relaxed charge-ordered model.     

X-ray directional dichroism of a polar ferrimagnet

In a polar ferrimagnet GaFeO3, we have found a novel magneto-optical effect, termed x-ray nonreciprocal directional dichroism (XNDD), that the x-ray absorption at around the K edge of an Fe ion depends on whether the x-ray propagation vector is parallel or antiparallel to the outer product of the magnetization and electric-polarization vectors. The XNDD spectroscopy as demonstrated here can be a useful tool to probe the local magnetism in noncentrosymmetric systems such as magnetic interfaces and nanostructures.     

Colossal magnetoresistance without phase separation: disorder-induced spin glass state and nanometer scale orbital-charge correlation in half doped manganites

The magnetic and electrical properties of high-quality single crystals of A-site disordered (solid solution) Ln0.5Ba0.5MnO3 are investigated near the phase boundary between the spin-glass insulator and colossal-magnetoresistive ferromagnetic metal, locating near Ln=Sm. The temperature dependence of the ac susceptibility and the x-ray diffuse scattering of Eu0.5Ba0.5MnO3 are analyzed in detail. The uniformity of the random potential perturbation in Ln0.5Ba0.5MnO3 crystals with a small bandwidth yields, rather than the phase separation, an homogeneous short ranged charge or orbital order which gives rise to a nearly atomic spin-glass state. Remarkably, this microscopically disordered "charge-exchange-glass" state alone is able to bring forth the colossal magnetoresistance.     

Magnetization-induced second harmonic generation in a polar ferromagnet

Second harmonic generation (SHG) induced by spontaneous magnetization has been investigated for a polar ferromagnetic crystal of GaFeO3. The Kerr rotation of the second harmonic light becomes gigantic with decreasing temperature below the magnetic transition temperature (approximately =205 K), e.g., as large as 73 degrees at 100 K. The magnetic domains can be visualized by using that large nonlinear Kerr rotation. The spectrum of the magnetization-induced SHG as measured indicates the two-photon resonant electronic process on a Fe3+ ion in the crystal.     

Change of electronic structure in Ca2RuO4 induced by orbital ordering

Optical conductivity spectra sigma(omega) were used to investigate the effect of orbital ordering on the electronic structure of Ca2RuO4. Our LDA+U calculation predicts Ru 4d(xy) ferro-orbital ordering at the ground state, and well explains the present sigma(omega) as well as the reported O 1s x-ray absorption spectra. Variation of temperature (T) causes a large change of spectral weight over several eV as well as collapse of a charge gap accompanied by elongation of the c-axis Ru-O bond length. These results clearly indicate that the d(xy) orbital ordering plays a crucial role in the metal-insulator transition and the T-dependent electronic structure on a large energy scale.