Metal-insulator transition and the Pr3+^{3+}/Pr4+^{4+} valence shift in (Pr1−y_{1-y}Yy_{y})0.7_{0.7}Ca0.3_{0.3}CoO3_3

The magnetic, electric and thermal properties of the ($Ln_{1-y}$Y$_{y}$)$_{0.7}$Ca$_{0.3}$CoO$_3$ perovskites ($Ln$~=~Pr, Nd) were investigated down to very low temperatures. The main attention was given to a peculiar metal-insulator transition, which is observed in the praseodymium based samples with $y=0.075$ and 0.15 at $T_{M-I}=64$ and 132~K, respectively. The study suggests that the transition, reported originally in Pr$_{0.5}$Ca$_{0.5}$CoO$_3$, is not due to a mere change of cobalt ions from the intermediate- to the low-spin states, but is associated also with a significant electron transfer between Pr$^{3+}$ and Co$^{3+}$/Co$^{4+}$ sites, so that the praseodymium ions occur below $T_{M-I}$ in a mixed Pr$^{3+}$/Pr$^{4+}$ valence. The presence of Pr$^{4+}$ ions in the insulating phase of the yttrium doped samples (Pr$_{1-y}$Y$_{y}$)$_{0.7}$Ca$_{0.3}$CoO$_3$ is evidenced by Schottky peak originating in Zeeman splitting of the ground state Kramers doublet. The peak is absent in pure Pr$_{0.7}$Ca$_{0.3}$CoO$_3$ in which metallic phase, based solely on non-Kramers Pr$^{3+}$ ions, is retained down to the lowest temperature.Comment: 10 figure

Synchronization of multi-phase oscillators: An Axelrod-inspired model

Inspired by Axelrod's model of culture dissemination, we introduce and analyze a model for a population of coupled oscillators where different levels of synchronization can be assimilated to different degrees of cultural organization. The state of each oscillator is represented by a set of phases, and the interaction --which occurs between homologous phases-- is weighted by a decreasing function of the distance between individual states. Both ordered arrays and random networks are considered. We find that the transition between synchronization and incoherent behaviour is mediated by a clustering regime with rich organizational structure, where some of the phases of a given oscillator can be synchronized to a certain cluster, while its other phases are synchronized to different clusters.Comment: 6 pages, 5 figure

Scaling of THz-conductivity at metal-insulator transition in doped manganites

Magnetic field and temperature dependence of the Terahertz conductivity and permittivity of the colossal magnetoresistance manganite Pr_{0.65}Ca_{0.28}Sr_{0.07}MnO_3 (PCSMO) is investigated approaching the metal-to-insulator transition (MIT) from the insulating side. In the charge-ordered state of PCSMO both conductivity and dielectric permittivity increase as function of magnetic field and temperature. Universal scaling relationships between the changes in permittivity and conductivity are observed in a broad range of temperatures and magnetic fields. Similar scaling is also seen in La_{1-x}Sr_xMnO_3 for different doping levels. The observed proportionality points towards the importance of pure ac-conductivity and phononic energy scale at MIT in manganites.Comment: 5 pages, 4 figure

Soft spin waves in the low temperature thermodynamics of Pr_{0.7}Ca_{0.3}MnO_{3}

We present a detailed magnetothermal study of Pr(0.7)Ca(0.3)MnO(3), a perovskite manganite in which an insulator-metal transition can be driven by magnetic field, but also by pressure, visible light, x-rays, or high currents. We find that the field-induced transition is associated with an enormous release of energy which accounts for its strong irreversibility. In the ferromagnetic metallic state, specific heat and magnetization measurements indicate a much smaller spin wave stiffness than that seen in any other manganite, which we attribute to spin waves among the ferromagnetically ordered Pr moments. The coupling between the Pr and Mn spins may also provide a basis for understanding the low temperature phase diagram of this most unusual manganite.Comment: 10 pages, LATEX, 5 PDF figures, corrected typo

Charge Ordering and Ferroelectricity in Half-doped Manganites

By means of density-functional simulations for half-doped manganites, such as pseudocubic Pr0.5Ca0.5MnO3 and bilayer PrCa2Mn2O7, we discuss the occurrence of ferroelectricity and we explore its crucial relation to the crystal structure and to peculiar charge/spin/orbital ordering effects. In pseudocubic Pr0.5Ca0.5MnO3, ferroelectricity is induced in the Zener polaron type structure, where Mn ions are dimerized. In marked contrast, in bilayer PrCa2Mn2O7, it is the displacements of apical oxygens bonded to either Mn3+ or Mn4+ ions that play a key role in the rising of ferroelectricity. Importantly, local dipoles due to apical oxygens are also intimately linked to charge and orbital ordering patterns in MnO2 planes, which in turn contribute to polarization. Finally, an important outcome of our work consists in proposing Born effective charges as a valid mean to quantify charge disproportionation effects, in terms of anisotropy and size of electronic clouds around Mn ions.Comment: 5 pages, 2 figures, submitted for publicatio

Hole-doping dependence of percolative phase separation in Pr_(0.5-delta)Ca_(0.2+delta)Sr_(0.3)MnO_(3) around half doping

We address the problem of the percolative phase separation in polycrystalline samples of Pr$_{0.5-\delta}$Ca$_{0.2+\delta}$Sr$_{0.3}$MnO$_3$ for $-0.04\leq \delta \leq 0.04$ (hole doping $n$ between 0.46 and 0.54). We perform measurements of X-ray diffraction, dc magnetization, ESR, and electrical resistivity. These samples show at $T_C$ a paramagnetic (PM) to ferromagnetic (FM) transition, however, we found that for $n>0.50$ there is a coexistence of both of these phases below $T_C$. On lowering $T$ below the charge-ordering (CO) temperature $T_{CO}$ all the samples exhibit a coexistence between the FM metallic and CO (antiferromagnetic) phases. In the whole $T$ range the FM phase fraction ($X$) decreases with increasing $n$. Furthermore, we show that only for $n\leq 0.50$ the metallic fraction is above the critical percolation threshold $X_C\simeq 15.5$. As a consequence, these samples show very different magnetoresistance properties. In addition, for $n\leq 0.50$ we observe a percolative metal-insulator transition at $T_{MI}$, and for $T_{MI}<T<T_{CO}$ the insulating-like behavior generated by the enlargement of $X$ with increasing $T$ is well described by the percolation law $\rho ^{-1}=\sigma \sim (X-X_C)^t$, where $t$ is a critical exponent. On the basis of the values obtained for this exponent we discuss different possible percolation mechanisms, and suggest that a more deep understanding of geometric and dimensionality effects is needed in phase separated manganites. We present a complete $T$ vs $n$ phase diagram showing the magnetic and electric properties of the studied compound around half doping.Comment: 9 text pages + 12 figures, submitted to Phys. Rev.

Anomalous field-dependent specific heat in charge-ordered Pr1−x_{1-x}Cax_xMnO3_3 and La0.5_{0.5}Ca0.5_{0.5}MnO3_3

We report low temperature specific heat measurements of Pr$_{1-x}$Ca$_{x}$MnO$_{3}$ ($0.3\leq x \leq 0.5$) and La$_{0.5}$Ca$_{0.5}$MnO$_{3}$ with and without applied magnetic field. An excess specific heat, $C^{\prime}(T)$, of non-magnetic origin associated with charge ordering is found for all the samples. A magnetic field sufficient to induce the transition from the charge-ordered state to the ferromagnetic metallic state does not completely remove the $C^{\prime}$ contribution. This suggests that the charge ordering is not completely destroyed by a "melting" magnetic field. In addition, the specific heat of the Pr$_{1-x}$Ca$_{x}$MnO$_{3}$ compounds exhibit a large contribution linear in temperature ($\gamma T$) originating from magnetic and charge disorder.Comment: submitted to PRL 5 pages, 3 figures include

Non-linear electrical response in a non-charge-ordered manganite: Pr0.8Ca0.2MnO3

Up to now, electric field induced non-linear conduction in the Pr(1-x)CaxMnO3 system has been ascribed to a current-induced destabilization of the charge ordered phase. However, for x<0.25, a ferromagnetic insulator state is observed and charge-ordering is absent whatever the temperature. A systematic investigation of the non-linear transport in the ferromagnetic insulator Pr0.8Ca0.2MnO3 shows rather similar results to those obtained in charge ordered systems. However, the experimental features observed in Pr0.8Ca0.2MnO3 are distinct in that the collapse of the CO energy gap can not be invoked as usually done in the other members of the PCMO system. We propose interpretations in which the effectiveness of the DE is restored upon application of electric field.Comment: 6 pages, 5 figure

The nanoscale phase separation in hole-doped manganites

A macroscopic phase separation, in which ferromagnetic clusters are observed in an insulating matrix, is sometimes observed, and believed to be essential to the colossal magnetoresistive (CMR) properties of manganese oxides. The application of a magnetic field may indeed trigger large magnetoresistance effects due to the percolation between clusters allowing the movement of the charge carriers. However, this macroscopic phase separation is mainly related to extrinsic defects or impurities, which hinder the long-ranged charge-orbital order of the system. We show in the present article that rather than the macroscopic phase separation, an homogeneous short-ranged charge-orbital order accompanied by a spin glass state occurs, as an intrinsic result of the uniformity of the random potential perturbation induced by the solid solution of the cations on the $A$-sites of the structure of these materials. Hence the phase separation does occur, but in a more subtle and interesting nanoscopic form, here referred as ``homogeneous''. Remarkably, this ``nanoscale phase separation'' alone is able to bring forth the colossal magnetoresistance in the perovskite manganites, and is potentially relevant to a wide variety of other magnetic and/or electrical properties of manganites, as well as many other transition metal oxides, in bulk or thin film form as we exemplify throughout the article.Comment: jpsj2 TeX style (J. Phys. Soc. Jpn); 18 pages, 7 figure

New Stacking Variations of the CE-type Structure in the Metal-Ordered Manganite YBaMn2O6

For the paramagnetic insulating phase in the metal-ordered manganite YBaMn2O6, the so-called CE-type of charge/orbital ordered state was observed within the monoclinic ab-plane, which is most commonly observed for the ordinary half doped manganites. However, TEM revealed a 4-fold periodicity along the c-axis, suggesting a new stacking pattern, where planes of the CE-type are built up according to the sequence [aabb...]. Interestingly, when th system enters into the antiferromagnetic state, this stacking pattern changes into [aaaa...] or [abab], suggesting close interplay between spins and orbitals. These features are discusses in terms of inherent structural alternation, i.e., the Y/Ba order along the c-axis.Comment: 13 pages, figures included, submitted to Journal of the Physical Society of Japa