Phonons and Magnetic Excitations in Mott-Insulator LaTiO3_3

The polarized Raman spectra of stoichiometric LaTiO$_3$ (T$_N = 150$ K) were measured between 6 and 300 K. In contrast to earlier report on half-metallic LaTiO$_{3.02}$, neither strong background scattering, nor Fano shape of the Raman lines was observed. The high frequency phonon line at 655 cm$^{-1}$ exhibits anomalous softening below T$_N$: a signature for structural rearrangement. The assignment of the Raman lines was done by comparison to the calculations of lattice dynamics and the nature of structural changes upon magnetic ordering are discussed. The broad Raman band, which appears in the antiferromagnetic phase, is assigned to two-magnon scattering. The estimated superexchange constant $J = 15.4\pm0.5$ meV is in excellent agreement with the result of neutron scattering studies.Comment: 4 pages, 5 figure

Determination of the orbital moment and crystal field splitting in LaTiO3_{3}

Utilizing a sum-rule in a spin-resolved photoelectron spectroscopic experiment with circularly polarized light, we show that the orbital moment in LaTiO$_3$ is strongly reduced both below and above the N\'{e}el temperature. Using Ti $L_{2,3}$ x-ray absorption spectroscopy as a local probe, we found that the crystal field splitting in the $t_{2g}$ subshell is about 0.12-0.30 eV. This large splitting does not facilitate the formation of an orbital liquid

Orbital order in the low-dimensional quantum spin system TiOCl probed by ESR

We present electron spin resonance data of Ti$^{3+}$ (3$d^1$) ions in single crystals of the novel layered quantum spin magnet TiOCl. The analysis of the g tensor yields direct evidence that the d_{xy} orbital from the t_{2g} set is predominantly occupied and owing to the occurrence of orbital order a linear spin chain forms along the crystallographic b axis. This result corroborates recent theoretical LDA+U calculations of the band structure. The temperature dependence of the parameters of the resonance signal suggests a strong coupling between spin and lattice degrees of freedom and gives evidence for a transition to a nonmagnetic ground state at 67 K.Comment: revised version, accepted for publication in Phys. Rev. B, Rapid Com

Crystal and magnetic structure of LaTiO3 : evidence for non-degenerate t2gt_{2g}-orbitals

The crystal and magnetic structure of LaTiO3 ~ has been studied by x-ray and neutron diffraction techniques using nearly stoichiometric samples. We find a strong structural anomaly near the antiferromagnetic ordering, T$_N$=146 K. In addition, the octahedra in LaTiO3 exhibit an intrinsic distortion which implies a splitting of the t2g-levels. Our results indicate that LaTiO3 should be considered as a Jahn-Teller system where the structural distortion and the resulting level splitting are enhanced by the magnetic ordering.Comment: 4 pages 5 figure

Hour-glass magnetic spectrum in an insulating, hole-doped antiferromagnet

Superconductivity in layered copper-oxide compounds emerges when charge carriers are added to antiferromagnetically-ordered CuO2 layers. The carriers destroy the antiferromagnetic order, but strong spin fluctuations persist throughout the superconducting phase and are intimately linked to super-conductivity. Neutron scattering measurements of spin fluctuations in hole-doped copper oxides have revealed an unusual `hour-glass' feature in the momentum-resolved magnetic spectrum, present in a wide range of superconducting and non-superconducting materials. There is no widely-accepted explanation for this feature. One possibility is that it derives from a pattern of alternating spin and charge stripes, an idea supported by measurements on stripe-ordered La1.875Ba0.125CuO4. However, many copper oxides without stripe order also exhibit an hour-glass spectrum$. Here we report the observation of an hour-glass magnetic spectrum in a hole-doped antiferromagnet from outside the family of superconducting copper oxides. Our system has stripe correlations and is an insulator, which means its magnetic dynamics can conclusively be ascribed to stripes. The results provide compelling evidence that the hour-glass spectrum in the copper-oxide superconductors arises from fluctuating stripes.Comment: 13 pages, 4 figures, to appear in Natur

Optical study of orbital excitations in transition-metal oxides

The orbital excitations of a series of transition-metal compounds are studied by means of optical spectroscopy. Our aim was to identify signatures of collective orbital excitations by comparison with experimental and theoretical results for predominantly local crystal-field excitations. To this end, we have studied TiOCl, RTiO3 (R=La, Sm, Y), LaMnO3, Y2BaNiO5, CaCu2O3, and K4Cu4OCl10, ranging from early to late transition-metal ions, from t_2g to e_g systems, and including systems in which the exchange coupling is predominantly three-dimensional, one-dimensional or zero-dimensional. With the exception of LaMnO3, we find orbital excitations in all compounds. We discuss the competition between orbital fluctuations (for dominant exchange coupling) and crystal-field splitting (for dominant coupling to the lattice). Comparison of our experimental results with configuration-interaction cluster calculations in general yield good agreement, demonstrating that the coupling to the lattice is important for a quantitative description of the orbital excitations in these compounds. However, detailed theoretical predictions for the contribution of collective orbital modes to the optical conductivity (e.g., the line shape or the polarization dependence) are required to decide on a possible contribution of orbital fluctuations at low energies, in particular in case of the orbital excitations at about 0.25 eV in RTiO3. Further calculations are called for which take into account the exchange interactions between the orbitals and the coupling to the lattice on an equal footing.Comment: published version, discussion of TiOCl extended to low T, improved calculation of orbital excitation energies in TiOCl, figure 16 improved, references updated, 33 pages, 20 figure

G-type antiferromagnetism and orbital ordering due to the crystal field from the rare-earth ions induced by the GdFeO_3-type distortion in RTiO_3 with R=La, Pr, Nd and Sm

The origin of the antiferromagnetic order and puzzling properties of LaTiO_3 as well as the magnetic phase diagram of the perovskite titanates are studied theoretically. We show that in LaTiO_3, the t_{2g} degeneracy is eventually lifted by the La cations in the GdFeO_3-type structure, which generates a crystal field with nearly trigonal symmetry. This allows the description of the low-energy structure of LaTiO_3 by a single-band Hubbard model as a good starting point. The lowest-orbital occupation in this crystal field stabilizes the AFM(G) state, and well explains the spin-wave spectrum of LaTiO_3 obtained by the neutron scattering experiment. The orbital-spin structures for RTiO_3 with R=Pr, Nd and Sm are also accounted for by the same mechanism. We point out that through generating the R crystal field, the GdFeO_3-type distortion has a universal relevance in determining the orbital-spin structure of the perovskite compounds in competition with the Jahn-Teller mechanism, which has been overlooked in the literature. Since the GdFeO_3-type distortion is a universal phenomenon as is seen in a large number of perovskite compounds, this mechanism may also play important roles in other compounds of this type.Comment: 20 pages, 15 figure

Dielectric properties and dynamical conductivity of LaTiO3: From dc to optical frequencies

We provide a complete and detailed characterization of the temperature-dependent response to ac electrical fields of LaTiO3, a Mott-Hubbard insulator close to the metal-insulator transition. We present combined dc, broadband dielectric, mm-wave, and infrared spectra of ac conductivity and dielectric constant, covering an overall frequency range of 17 decades. The dc and dielectric measurements reveal information on the semiconducting charge-transport properties of LaTiO3, indicating the importance of Anderson localization, and on the dielectric response due to ionic polarization. In the infrared region, the temperature dependence of the phonon modes gives strong hints for a structural phase transition at the magnetic ordering temperature. In addition, a gap-like electronic excitation following the phonon region is analyzed in detail. We compare the results to the soft-edge behavior of the optical spectra characteristic for Mott-Hubbard insulators. Overall a consistent picture of the charge-transport mechanisms in LaTiO3 emerges.Comment: 11 pages, 8 figures, 1 tabl