Simultaneous valence shift of Pr and Tb ions at the spin-state transition in ((Pr1−y_{1-y}Tby)0.7_{y})_{0.7}Ca0.3_{0.3}CoO3_{3}

Temperature dependence of the X-ray absorption near-edge structure (XANES) spectra at the Pr $L_{3}$- and Tb $L_{3}$-edges was measured for the (Pr$_{1-y}$Tb$_{y})_{0.7}$Ca$_{0.3}$CoO$_{3}$ system, in which a metal-insulator (MI) and spin-state (SS) transition took place simultaneously at a critical temperature $T_{\rm MI}$. A small increase in the valence of the terbium ion was found below $T_{\rm MI}$, besides the enhancement of the praseodymium valence; the trivalent states, which are stable at room temperature, change to a 3+/4+ ionic mixture at low temperatures. In particular for the $y$=0.2 sample, the average valence determined at 8 K amounts to 3.03+ and 3.25+ for the Tb and Pr ion, respectively. In analogous (Pr$_{1-y}$RE$_{y})_{0.7}$Ca$_{0.3}$CoO$_{3}$ samples (RE=Sm and Eu), in which the MI-SS transition also took place, no valence shift of the RE ion was detected in the XANES spectra at the RE ion $L_{3}$-edge. The role of the substituted RE ion for the Pr-site on the MI-SS transition is discussed

Microphase separation in Pr0.67Ca0.33MnO3 by small angle neutron scattering

We have evidenced by small angle neutron scattering at low temperature the coexistence of ferromagnetism (F) and antiferromagnetism (AF) in Pr0.67Ca0.33MnO3. The results are compared to those obtained in Pr0.80Ca0.20MnO3 and Pr0.63Ca0.37MnO3, which are F and AF respectively. Quantitative analysis shows that the small angle scattering is not due to a mesoscopic mixing but to a nanoscopic electronic and magnetic ''red cabbage'' structure, in which the ferromagnetic phase exists in form of thin layers in the AF matrix (stripes or 2D ''sheets'').Comment: 4 figure

Charge and Orbital Ordering in Pr_{0.5} Ca_{0.5} MnO_3 Studied by ^{17}O NMR

The charge and orbital ordering in Pr_{0.5} Ca_{0.5} MnO_3 is studied for the first time by ^{17}O NMR. This local probe is sensitive to spin, charge and orbital correlations. Two transitions exist in this system: the charge and orbital ordering at T_{CO} = 225 K and the antiferromagnetic (AF) transition at T_N = 170 K. Both are clearly seen in the NMR spectra measured in a magnetic field of 7T. Above T_{CO} there exists only one NMR line with a large isotropic shift, whose temperature dependence is in accordance with the presence of ferromagnetic (FM) correlations. This line splits into two parts below T_{CO}, which are attributed to different types of oxygen in the charge/orbital ordered state. The interplay of FM and AF spin correlations of Mn ions in the charge ordered state of Pr_{0.5} Ca_{0.5} MnO_3 is considered in terms of the hole hopping motion that is slowed down with decreasing temperature. The developing fine structure of the spectra evidences, that there still exist charge-disordered regions at T_{CO} > T > T_N and that the static (t > 10^{-6}s) orbital order is established only on approaching T_N. The CE-type magnetic correlations develop gradually below T_{CO}, so that at first the AF correlations between checkerboard ab-layers appear, and only at lower temperature - CE correlations within the ab-planes

Phase separation, percolation and giant isotope effect in manganites

Phase separation and a tendency to form inhomogeneous structures seems to be a generic property of systems with strongly correlated electrons. After shortly summarising the existing theoretical results in this direction, I concentrate on the phenomena in doped manganites. I discuss general theoretical results on the phase separation at small doping and close to the doping x=0.5. The "global" phase diagram in this region is constructed. These general results are illustrated on the example of the particular system with rich and complicated properties - (LaPr)_(1-x)Ca_xMnO_3 in which there exist a ferromagnetic metallic (FM) phase and a charge ordered (CO) insulating one. The experimental situation in this system is discussed and the interpretation is given in the framework of the model with competition of FM and CO, and the indications of phase separation and percolative nature of this system are given. Giant isotope effect observed in this situation is shortly discussed.Comment: 7 pages, 5 eps figures, uses elsart.cls and phbauth.cls, invited talk at the LT22, Helsinki 199

Competition between ferromagnetic and charge-orbital ordered phases in Pr1−x_{1-x}Cax_{x}MnO3_3 for xx=1/4, 3/8, and 1/2

Spin, charge, and orbital structures in models for doped manganites are studied by a combination of analytic mean-field and numerical relaxation techniques. At realistic values for the electron-phonon and antiferromagnetic $t_{2g}$ spin couplings, a competition between a ferromagnetic (FM) phase and a charge-orbital ordered (COO) insulating state is found for $x$=1/4, 3/8, and 1/2, as experimentally observed in Pr$_{1-x}$Ca$_{x}$MnO$_3$ for $x$=0.3$\sim$0.5. The theoretical predictions for the spin-charge-orbital ordering pattern are compared with experiments. The FM-COO energy difference is surprisingly small for the densities studied, result compatible with the presence of a robust colossal-magnetoresistive effect in Pr$_{1-x}$Ca$_{x}$MnO$_3$ in a large density interval.Comment: 4 pages, Revtex, with 2 figures embedded in the text. Submitted to Phys. Rev.

Phase Separation and the Low-Field Bulk Magnetic Properties of Pr0.7Ca0.3MnO3

We present a detailed magnetic study of the perovskite manganite Pr0.7Ca0.3MnO3 at low temperatures including magnetization and a.c. susceptibility measurements. The data appear to exclude a conventional spin glass phase at low fields, suggesting instead the presence of correlated ferromagnetic clusters embedded in a charge-ordered matrix. We examine the growth of the ferromagnetic clusters with increasing magnetic field as they expand to occupy almost the entire sample at H ~ 0.5 T. Since this is well below the field required to induce a metallic state, our results point to the existence of a field-induced ferromagnetic insulating state in this material.Comment: 15 pages with figures, submitted to Physical Review

Field dependence of the electronic phase separation in Pr0.67Ca0.33MnO3 by small angle magnetic neutron scattering

We have studied by small angle neutron scattering the evolution induced by the application of magnetic field of the coexistence of ferromagnetism (F) and antiferromagnetism (AF) in a crystal of Pr$_{0.67}$Ca$_{0.33}$MnO$_3$. The results are compared to magnetic measurements which provide the evolution of the ferromagnetic fraction. These results show that the growth of the ferromagnetic phase corresponds to an increase of the thickness of the ferromagnetic ''cabbage'' sheets

Orbital polarons and ferromagnetic insulators in manganites

We argue that in lightly hole doped perovskite-type Mn oxides the holes (Mn$^{4+}$ sites) are surrounded by nearest neighbor Mn$^{3+}$ sites in which the occupied $3d$ orbitals have their lobes directed towards the central hole (Mn$^{4+}$) site and with spins coupled ferromagnetically to the central spin. This composite object, which can be viewed as a combined orbital-spin-lattice polaron, is accompanied by the breathing type (Mn$^{4+}$) and Jahn-Teller type (Mn$^{3+}$) local lattice distortions. We present calculations which indicate that for certain doping levels these orbital polarons may crystallize into a charge and orbitally ordered ferromagnetic insulating state.Comment: 5 pages, 4 figures, to be published in PR

Multiphase segregation and metal-insulator transition in single crystal La(5/8-y)Pr(y)Ca(3/8)MnO3

The insulator-metal transition in single crystal La(5/8-y)Pr(y)Ca(3/8)MnO3 with y=0.35 was studied using synchrotron x-ray diffraction, electric resistivity, magnetic susceptibility, and specific heat measurements. Despite the dramatic drop in the resistivity at the insulator-metal transition temperature Tmi, the charge-ordering (CO) peaks exhibit no anomaly at this temperature and continue to grow below Tmi. Our data suggest then, that in addition to the CO phase, another insulating phase is present below Tco. In this picture, the insulator-metal transition is due to the changes within this latter phase. The CO phase does not appear to play a major role in this transition. We propose that a percolation-like insulator-metal transition occurs via the growth of ferromagnetic metallic domains within the parts of the sample that do not exhibit charge ordering. Finally, we find that the low-temperature phase-separated state is unstable against x-ray irradiation, which destroys the CO phase at low temperatures.Comment: 9 pages, 9 encapsulated eps figure

Polarization Dependence of Anomalous X-ray Scattering in Orbital Ordered Manganites

In order to determine types of the orbital ordering in manganites, we study theoretically the polarization dependence of the anomalous X-ray scattering which is caused by the anisotropy of the scattering factor. The general formulae of the scattering intensity in the experimental optical system is derived and the atomic scattering factor is calculated in the microscopic electronic model. By using the results, the X-ray scattering intensity in several types of the orbital ordering is numerically calculated as a function of azimuthal and analyzer angles.Comment: 9 pages, 7 figure