Fingerprints of Mott-Hubbard physics in optical spectra of antiferromagnetic LaTiO3

Magnetic properties of Mott-Hubbard insulators are determined by superexchange interactions mediated by the high-spin (HS) and low-spin (LS) intersite d-d charge excitations, which can be associated with the HS- and LS-Hubbard subbands in optical experiments. To explore the Mott-Hubbard physics in orthorhombic LaTiO_3 crystal exhibiting the G-type antiferromagnetic order at the Neel temperature T_N = 146 K, we present a comprehensive spectroscopic ellipsometry study in the spectral range 0.5-5.6 eV at temperatures 10 K < T < 300 K. We found that the complex dielectric function spectra of LaTiO_3 crystal are almost featureless, nearly isotropic, and weakly temperature dependent in the range of d-d optical transitions. Nonetheless, analyzing the difference spectra below the T_N, we have identified the LS-state d^1d^1 - d^2d^0 excitations at ~3.7 and ~5.15 eV and estimated values of the on-site Coulomb repulsion U ~4.2 eV and Hund's exchange constant J_H ~0.5 eV, which define the energy of the HS-state d^1d^1 - d^2d^0 excitation at ~2.7 eV. In addition, we discovered that the pronounced lowest-energy 1.3 eV optical band displays the critical intensity behavior and anomalous broadening with decreasing temperature below the T_N. The discovered properties indicate that the 1.3 eV band in LaTiO_3 can be associated with a Mott-Hubbard exciton.Comment: 8 pages, 8 figures, 1 tabl

Giant phonon anomalies in the pseudo-gap phase of TiOCl

We report infrared and Raman spectroscopy results of the spin-1/2 quantum magnet TiOCl. Giant anomalies are found in the temperature dependence of the phonon spectrum, which hint to unusual coupling of the electronic degrees of freedom to the lattice. These anomalies develop over a broad temperature interval, suggesting the presence of an extended fluctuation regime. This defines a pseudo-gap phase, characterized by a local spin-gap. Below 100 K a dimensionality cross-over leads to a dimerized ground state with a global spin-gap of about 2$\Delta_{spin}\approx$~430 K.Comment: 4 pages, 3 figures, for further information see http://www.peter-lemmens.d

Formation of metallic magnetic clusters in a Kondo-lattice metal: Evidence from an optical study

Magnetic materials are usually divided into two classes: those with localised magnetic moments, and those with itinerant charge carriers. We present a comprehensive experimental (spectroscopic ellipsomerty) and theoretical study to demonstrate that these two types of magnetism do not only coexist but complement each other in the Kondo-lattice metal, Tb2PdSi3. In this material the itinerant charge carriers interact with large localised magnetic moments of Tb(4f) states, forming complex magnetic lattices at low temperatures, which we associate with self-organisation of magnetic clusters. The formation of magnetic clusters results in low-energy optical spectral weight shifts, which correspond to opening of the pseudogap in the conduction band of the itinerant charge carriers and development of the low- and high-spin intersite electronic transitions. This phenomenon, driven by self-trapping of electrons by magnetic fluctuations, could be common in correlated metals, including besides Kondo-lattice metals, Fe-based and cuprate superconductors.Comment: 30 pages, 6 Figure

In-Plane Spectral Weight Shift of Charge Carriers in YBa2Cu3O6.9YBa_2Cu_3O_{6.9}

The temperature dependent redistribution of the spectral weight of the $CuO_2$ plane derived conduction band of the $YBa_2Cu_3O_{6.9}$ high temperature superconductor (T_c = 92.7 K) was studied with wide-band (from 0.01 to 5.6 eV) spectroscopic ellipsometry. A superconductivity - induced transfer of the spectral weight involving a high energy scale in excess of 1 eV was observed. Correspondingly, the charge carrier spectral weight was shown to decrease in the superconducting state. The ellipsometric data also provide detailed information about the evolution of the optical self-energy in the normal and superconducting states

Infrared studies of a La_(0.67)Ca_(0.33)MnO_3 single crystal: Optical magnetoconductivity in a half-metallic ferromagnet

The infrared reflectivity of a La_(0.67)Ca_(0.33)MnO_3 single crystal is studied over a broad range of temperatures (78–340 K), magnetic fields (0–16 T), and wave numbers (20–9000cm^(-1)). The optical conductivity gradually changes from a Drude-like behavior to a broad peak feature near 5000cm-1 in the ferromagnetic state below the Curie temperature T_C=307K. Various features of the optical conductivity bear striking resemblance to recent theoretical predictions based on the interplay between the double exchange interaction and the Jahn-Teller electron-phonon coupling. A large optical magnetoconductivity is observed near T_C

Infrared Studies of a La_{0.67}Ca_{0.33}MnO_3 Single Crystal: Optical Magnetoconductivity in a Half-Metallic Ferromagnet

The infrared reflectivity of a $\rm La_{0.67}Ca_{0.33}MnO_3$ single crystal is studied over a broad range of temperatures (78-340 K), magnetic fields (0-16 T), and wavenumbers (20-9000 cm$^{-1}$). The optical conductivity gradually changes from a Drude-like behavior to a broad peak feature near 5000 cm$^{-1}$ in the ferromagnetic state below the Curie temperature $T_C=307 K$. Various features of the optical conductivity bear striking resemblance to recent theoretical predictions based on the interplay between the double exchange interaction and the Jahn-Teller electron-phonon coupling. A large optical magnetoconductivity is observed near $T_C$.Comment: 4 pages, 4 figures, Latex, PostScript; The 7th Joint MMM-Intermag Conference,San Francisco, January 6-9, 1998; The Int. Conf. on Strongly Correlated Electron Systems, Paris, July 15-18,199

Low-energy Mott-Hubbard excitations in LaMnO_3 probed by optical ellipsometry

We present a comprehensive ellipsometric study of an untwinned, nearly stoichiometric LaMnO_3 crystal in the spectral range 1.2-6.0 eV at temperatures 20 K < T < 300 K. The complex dielectric response along the b and c axes of the Pbnm orthorhombic unit cell, \epsilon^b(\nu) and \epsilon^c(\nu), is highly anisotropic over the spectral range covered in the experiment. The difference between \epsilon^b(\nu) and \epsilon^c(\nu) increases with decreasing temperature, and the gradual evolution observed in the paramagnetic state is strongly enhanced by the onset of A-type antiferromagnetic long-range order at T_N = 139.6 K. In addition to the temperature changes in the lowest-energy gap excitation at 2 eV, there are opposite changes observed at higher energy at 4 - 5 eV, appearing on a broad-band background due to the strongly dipole-allowed O 2p -- Mn 3d transition around the charge-transfer energy 4.7 eV. Based on the observation of a pronounced spectral-weight transfer between low- and high-energy features upon magnetic ordering, they are assigned to high-spin and low-spin intersite d^4d^4 - d^3d^5 transitions by Mn electrons. The anisotropy of the lowest-energy optical band and the spectral weight shifts induced by antiferromagnetic spin correlations are quantitatively described by an effective spin-orbital superexchange model. An analysis of the multiplet structure of the intersite transitions by Mn e_g electrons allowed us to estimate the effective intra-atomic Coulomb interaction, the Hund exchange coupling, and the Jahn-Teller splitting energy between e_g orbitals in LaMnO_3. This study identifies the lowest-energy optical transition at 2 eV as an intersite d-d transition, whose energy is substantially reduced compared to that obtained from the bare intra-atomic Coulomb interaction.Comment: 10 pages, 14 figure