Suppressed Coherence due to Orbital Correlations in the Ferromagnetically Ordered Metallic Phase of Mn Compounds

Small Drude weight $D$ together with small specific heat coefficient $\gamma$ observed in the ferromagnetic phase of R$_{1-x}$A$_x$MnO$_3$ (R=La, Pr, Nd, Sm; A=Ca, Sr, Ba) are analyzed in terms of a proximity effect of the Mott insulator. The scaling theory for the metal-insulator transition with the critical enhancement of orbital correlations toward the staggered ordering of two $e_g$ orbitals such as $3x^2-r^2$ and $3y^2-r^2$ symmetries may lead to the critical exponents of $D \propto \delta^{u}$ and $\gamma \propto \delta^v$ with $u=3/2$ and $v=0$. The result agrees with the experimental indications.Comment: 4 pages LaTeX using jpsj.sty. To appear in J. Phys. Soc. Jpn. 67(1998)No.

One-Center Charge Transfer Transitions in Manganites

In frames of a rather conventional cluster approach, which combines the crystal field and the ligand field models we have considered different charge transfer (CT) states and O 2p-Mn 3d CT transitions in MnO$_{6}^{9-}$ octahedra. The many-electron dipole transition matrix elements were calculated using the Racah algebra for the cubic point group. Simple "local" approximation allowed to calculate the relative intensity for all dipole-allowed $\pi -\pi$ and $\sigma -\sigma$ CT transitions. We present a self-consistent description of the CT bands in insulating stoichiometric LaMn$^{3+}$O$_3$ compound with the only Mn$^{3+}$ valent state and idealized octahedral MnO$_{6}^{9-}$ centers which allows to substantially correct the current interpretation of the optical spectra. Our analysis shows the multi-band structure of the CT optical response with the weak low-energy edge at 1.7 eV, associated with forbidden $t_{1g}(\pi)-e_{g}$ transition and a series of the weak and strong dipole-allowed high-energy transitions starting from 2.5 and 4.5 eV, respectively, and extending up to nearly 11 eV. The most intensive features are associated with two strong composite bands near $4.6\div 4.7$ eV and $8\div 9$ eV, respectively, resulting from the superposition of the dipole-allowed $\sigma -\sigma$ and $\pi -\pi$ CT transitions. These predictions are in good agreement with experimental spectra. The experimental data point to a strong overscreening of the crystal field parameter $Dq$ in the CT states of MnO$_{6}^{9-}$ centers.Comment: 10 pages, 3 figure

Optical conductivity in doped manganites with planar x2^2-y2^2 orbital order

We investigate a planar model for the ferromagnetic (FM) phase of manganites, which develops orbital order of $e_g$ electrons with x$^2$-y$^2$-symmetry at low temperature. The dynamic structure factor of orbital excitations and the optical conductivity $\sigma(\omega)$ are studied with help of a finite-temperature diagonalization method. Our calculations provide a theoretical prediction for $\sigma(\omega)$ for the 2D FM state and are of possible relevance for the recently found A-type phase of manganites at high doping which consists of FM layers coupled antiferromagnetically. In the x$^2$-y$^2$ ordered regime $\sigma(\omega)$ shows both a Drude peak and a gapped incoherent absorption due to a gap in the orbital excitations.Comment: 5 pages, 5 figures, to appear in Phys. Rev. Let

Dimensional Crossover driven by Magnetic Ordering in Optical Conductivity of Pr_{1/2}Sr_{1/2}MnO_3

We investigated optical properties of Pr_{0.5}Sr_{0.5}MnO_3, which has the A-type antiferromagnetic ordering at a low temperature. We found that T- dependence of spectral weight transfer shows a clear correlation with the magnetic phase transition. In comparison with the optical conductivity results of Nd_{0.5}Sr_{0.5}MnO_3, which has the CE-type antiferromagnetic charge ordering, we showed that optical properties of Pr_{0.5}Sr_{0.5}MnO_3 near the Neel temperature could be explained by a crossover from 3D to 2D metals. Details of spectral weight changes are consistent with the polaron picture.Comment: 11 pages, 4 figures, submitted to PRL at June

Ultrafast Photoinduced Formation of Metallic State in a Perovskite-type Manganite with Short Range Charge and Orbital Order

Femtosecond reflection spectroscopy was performed on a perovskite-type manganite, Gd0.55Sr0.45MnO3, with the short-range charge and orbital order (CO/OO). Immediately after the photoirradiation, a large increase of the reflectivity was detected in the mid-infrared region. The optical conductivity spectrum under photoirradiation obtained from the Kramers-Kronig analyses of the reflectivity changes demonstrates a formation of a metallic state. This suggests that ferromagnetic spin arrangements occur within the time resolution (ca. 200 fs) through the double exchange interaction, resulting in an ultrafast CO/OO to FM switching.Comment: 4 figure

Spin/Orbital Pattern-Dependent Polaron Absorption in Nd(1-x)Sr(x)MnO3

We investigated optical properties of Nd(1-x)Sr(x)MnO3 (x= 0.40, 0.50, 0.55, and 0.65) single crystals. In the spin/orbital disordered state, their conductivity spectra look quite similar, and the strength of the mid-infrared absorption peak is proportional to x(1-x) consistent with the polaron picture. As temperature lowers, the Nd(1-x)Sr(x)MnO3 samples enter into various spin/orbital ordered states, whose optical responses are quite different. These optical responses can be explained by the spin/orbital ordering pattern-dependent polaron hopping.Comment: 3 figures (gzipped

Incoherent Charge Dynamics in Perovskite Manganese Oxides

A minimal model is proposed for the perovskite manganese oxides showing the strongly incoherent charge dynamics with a suppressed Drude weight in the ferromagnetic and metallic phase near the insulator. We investigate a generalized double-exchange model including three elements; the orbital degeneracy of $e_g$ conduction bands, the Coulomb interaction and fluctuating Jahn-Teller distortions. We demonstrate that Lancz$\ddot{\rm o}$s diagonalization calculations combined with Monte Carlo sampling of the largely fluctuating lattice distortions result in the optical conductivity which quantitatively accounts for the experimental indications. It is found that all the three elements are indispensable to understand the charge dynamics in these compounds.Comment: 4 pages with 1 page of figures. To appear in J. Phys. Soc. Jp

Dynamic conductivity of semiconducting manganites approaching the metal-insulator transition

We report the frequency-dependent conductivity of the manganite system La1-xSrxMnO3 (x <= 0.2) when approaching the metal-insulator transition from the insulating side. Results from low-frequency dielectric measurements are combined with spectra in the infrared region. For low doping levels the behavior is dominated by hopping transport of localized charge carriers at low frequencies and by phononic and electronic excitations in the infrared region. For the higher Sr contents the approach of the metallic state is accompanied by the successive suppression of the hopping contribution at low frequencies and by the development of polaronic excitations in the infrared region, which finally become superimposed by a strong Drude contribution in the fully metallic state.Comment: 10 pages, 7 figure

Effects of Orbital Degeneracy and Electron Correlation on Charge Dynamics in Perovskite Manganese Oxides

Taking the orbital degeneracy of $e_g$ conduction bands and the Coulomb interaction into account in a double-exchange model, we investigate charge dynamics of perovskite Mn oxides by the Lancz$\ddot{\rm o}$s diagonalization method. In the metallic phase near the Mott insulator, it is found that the optical conductivity for a spin-polarized two-dimensional system exhibits a weight transfer to a broad and incoherent structure within the lower-Hubbard band together with a suppressed Drude weight. It reproduces qualitative feature of the experimental results. As an orbital effect, we find that an anomalous charge correlation at quarter filling suppresses the coherent charge dynamics and signals precursor to the charge ordering.Comment: 4 pages LaTeX including 3 PS figures, to appear in J. Phys. Soc. Jp