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 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

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.

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

Formation of finite antiferromagnetic clusters and the effect of electronic phase separation in Pr{_0.5}Ca{_0.5}Mn{_0.975}Al{_0.025}O{_3}

We report the first experimental evidence of a magnetic phase arising due to the thermal blocking of antiferromagnetic clusters in the weakened charge and orbital ordered system Pr{_0.5}Ca{_0.5}Mn{_0.975}Al{_0.025}O{_3}. The third order susceptibility (\chi_3) is used to differentiate this transition from a spin or cluster glass like freezing mechanism. These clusters are found to be mesoscopic and robust to electronic phase separation which only enriches the antiphase domain walls with holes at the cost of the bulk, without changing the size of these clusters. This implies that Al substitution provides sufficient disorder to quench the length scales of the striped phases.Comment: 4 Post Script Figure

X-ray Resonant Scattering Studies of Orbital and Charge Ordering in Pr1−x_{1-x}Cax_xMnO3_3

We present the results of a systematic x-ray scattering study of the charge and orbital ordering in the manganite series Pr$_{1-x}$Ca$_x$MnO$_3$ with $x$=0.25, 0.4 and 0.5. The temperature dependence of the scattering at the charge and orbital wavevectors, and of the lattice constants, was characterized throughout the ordered phase of each sample. It was found that the charge and orbital order wavevectors are commensurate with the lattice, in striking contrast to the results of earlier electron diffraction studies of samples with $x$=0.5. High momentum-transfer resolution studies of the x=0.4 and 0.5 samples further revealed that while long-range charge order is present, long-range orbital order is never established. Above the charge/orbital ordering temperature T$_o$, the charge order fluctuations are more highly correlated than the orbital fluctuations. This suggests that charge order drives orbital order in these samples. In addition, a longitudinal modulation of the lattice with the same periodicity as the charge and orbital ordering was discovered in the x=0.4 and 0.5 samples. For x=0.25, only long-range orbital order was observed with no indication of charge ordering, nor of an additional lattice modulation. We also report the results of a preliminary investigation of the loss of charge and orbital ordering in the x=0.4 sample by application of a magnetic field. Finally, the polarization and azimuthal dependence of the charge and orbital ordering in these compounds is characterized both in the resonant and nonresonant limits, and compared with the predictions of current theories. The results are qualitatively consistent with both cluster and LDA+U calculations of the electronic structure.Comment: 37 pages, 22 figure