Charge, Orbital and Magnetic Order in Nd0.5Ca0.5MnO3

In the manganite Nd0.5Ca0.5MnO3, charge ordering occurs at much higher temperature than the antiferromagnetic order (TCO=250K,TN=160K). The magnetic behavior of the phase TN<T<TCO is puzzling: its magnetization and susceptibility are typical of an antiferromagnet while no magnetic order is detected by neutron diffraction.We have undertaken an extensive study of the cristallographic, electric and magnetic properties of Nd0.5Ca0.5MnO3 and established its phase diagram as a function of temperature and magnetic field. The charge disordered, paramagnetic phase above TCO present ferromagnetic correlations. An antiferromagnetic CE phase prevails below TN, with complete charge and orbital ordering. In the intermediate temperature range, charge ordering occurs while orbital ordering sets in progressively, with no magnetic order. Strong magnetic fields destroy the charge ordered phases in a fisrt order transition towards a ferromagnetic state.Comment: 17 pages, 11 Figures to appear in Phys. Rev.

Influence of Nd on the magnetic properties of Nd1-xCaxMnO3

The role played by the Nd ions in the magnetic properties of Nd0.5Ca0.5MnO3 and Nd0.7Ca0.3MnO3 is studied using static magnetization, neutron diffraction and high frequency (9.4-475GHz) Electron Spin Resonance. We show that the Nd ions are weakly coupled to the Mn ions via ferromagnetic exchange and are responsible for the peculiar ferromagnetic resonance observed in the FM phase of both compounds (ground state below 120K for x=0.3, high field state for x=0.5). We then use ESR to look for magnetic phase separation in the low field, CO phase of Nd0.5Ca0.5MnO3. We show that there is no trace of the FM phase imbedded in the CO phase, contrary to what is observed in La0.5Ca0.5MnO3 or Pr0.5Sr0.5MnO3.Comment: to be published in phys.Rev.B as a Rapid Com

Structures and Electromagnetic Properties of New Metal-Ordered Manganites; RBaMn_{2}O_{6} (R = Y and Rare Earth Elements)

New metal-ordered manganites RBaMn_{2}O_{6} have been synthesized and investigated in the structures and electromagnetic properties. RBaMn_{2}O_{6} can be classified into three groups from the structural and electromagnetic properties. The first group (R = La, Pr and Nd) has a metallic ferromagnetic transition, followed by an A-type antiferromagnetic transition in PrBaMn_{2}O_{6}. The second group (R = Sm, Eu and Gd) exhibits a charge-order transition, followed by an antiferromagnetic long range ordering. The third group (R = Tb, Dy and Ho) shows successive three phase transitions, the structural, charge/orbital-order and magnetic transitions, as observed in YBaMn_{2}O_{6}. Comparing to the metal-disordered manganites (R^{3+}_{0.5}A^{2+}_{0.5})MnO_{3}, two remarkable features can be recognized in RBaMn_{2}O_{6}; (1) relatively high charge-order transition temperature and (2) the presence of structural transition above the charge-order temperature in the third group. We propose a possible orbital ordering at the structural transition, that is a possible freezing of the orbital, charge and spin degrees of freedom at the independent temperatures in the third group. These features are closely related to the peculiar structure that the MnO_{2} square-lattice is sandwiched by the rock-salt layers of two kinds, RO and BaO with extremely different lattice-sizes.Comment: 5 pages, 4 figures, submitted to J. Phys. Soc. Jp

Electron- and Hole-Doping Effects on AA-site Ordered NdBaMn2_2O6_6

We have investigated electron- and hole-doping effects on $A$-site ordered perovskite manganite NdBaMn$_2$O$_6$, which has the $A$-type (layered) antiferromagnetic (AFM) ground state. Electrons (holes) are introduced by partial substitution of Ba$^{2+}$ (Nd$^{3+}$) with Nd$^{3+}$ (Ba$^{2+}$). Electron-doping generates ferromagnetic (FM) clusters in the $A$-type AFM matrix. With increasing the electron-doping level, the volume fraction of the FM phase or the number of the FM clusters is abruptly increasing. In contrast, the $A$-type AFM phase is robust against the hole-doping, and no FM correlation is observed in the hole-doped NdBaMn$_2$O$_6$.Comment: 8 pages, 5 figures, to be published in Journal of the Physical Society of Japa

A-site Randomness Effect on Structural and Physical Properties of Ba-based Perovskite Manganites

The discovery of novel structural and physical properties in the $A$-site ordered manganite $R$BaMn$_{2}$O$_{6}$ ($R$ = Y and rare earth elements) has demanded new comprehension about perovskite manganese oxides. In the present study, the $A$-site disordered form, $R_{0.5}$Ba$_{0.5}$MnO$_{3}$, has been investigated and compared with both $R$BaMn$_{2}$O$_{6}$ and $R_{0.5}A_{0.5}$MnO$_{3}$ ($A$: Sr, Ca) in the structures and electromagnetic properties. $R_{0.5}$Ba$_{0.5}$MnO$_{3}$ has a primitive cubic perovskite cell in the structure and magnetic glassy states are dominant as its ground state, in contrast to the ordinary disordered $R_{0.5}A_{0.5}$MnO$_{3}$ ($A$: Sr, Ca). In Pr-compounds with various degrees of Pr/Ba randomness at the $A$-sites, the $A$-site disorder gradually suppresses both ferromagnetic and A-type antiferromagnetic transitions and finally leads to a magnetic glassy state in Pr$_{0.5}$Ba$_{0.5}$MnO$_{3}$. A peculiar behavior, multi-step magnetization and resistivity change, has been observed in Pr$_{0.5}$Ba$_{0.5}$MnO$_{3}$. These properties could be closely related to any spatial heterogeneity caused by the random distribution of Ba$^{2 +}$ and $R^{3 +}$ with much different ionic radius.Comment: 9 pages, to be published in J. Phys. Soc. Jpn. 73 Aug. (2004

Pressure induced transition from a spin glass to an itinerant ferromagnet in half doped manganite Ln0.5Ba0.5MnO3 (Ln=Sm and Nd) with quenched disorder

The effect of quenched disorder on the multiphase competition has been investigated by examining the pressure phase diagram of half doped manganite Ln0.5B0.5MnO3 (Ln = Sm and Nd) with A-site disorders. Sm0.5Ba0.5MnO3, a spin glass insulator at ambient pressure, switches to a ferromagnetic metal with increasing pressure, followed by a rapid increase of the ferromagnetic transition temperature Tc. The rapid increase of Tc was confirmed also for Nd0.5Ba0.5MnO3. These observations indicate that the unusual suppression of the multicritical phase boundary in the A-site disordered system, previously observed as a function of the averaged A-site ionic radius, is essentially controlled by the pressure and hence the band width. The effect of quenched disorder is therefore much enhanced with approaching the multicritical region.Comment: 4 pages including 3 figure

Charge and Orbital Ordering and Spin State Transition Driven by Structural Distortion in YBaCo_2O_5

We have investigated electronic structures of antiferromagnetic YBaCo_2O_5 using the local spin-density approximation (LSDA) + U method. The charge and orbital ordered insulating ground state is correctly obtained with the strong on-site Coulomb interaction. Co^{2+} and Co^{3+} ions are found to be in the high spin (HS) and intermediate spin (IS) state, respectively. It is considered that the tetragonal to orthorhombic structural transition is responsible for the ordering phenomena and the spin states of Co ions. The large contribution of the orbital moment to the total magnetic moment indicates that the spin-orbit coupling is also important in YBaCo_2O_5.Comment: 4 pages including 4 figures, Submitted to Phys. Rev. Let

Specific heat and magnetic measurements in Nd0.5Sr0.5MnO3, Nd0.5Ca0.5MnO3 and Ho0.5Ca0.5MnO3 samples

We studied the magnetization as a function of temperature and magnetic field in the compounds Nd0.5Sr0.5MnO3, Nd0.5Ca0.5MnO3 and Ho0.5Ca0.5MnO3. It allowed us to identify the ferromagnetic, antiferromagnetic and charge ordering phases in each case. The intrinsic magnetic moments of Nd3+ and Ho3+ ions experienced a short range order at low temperatures. We also did specific heat measurements with applied magnetic fields between 0 and 9 T and temperatures between 2 and 300 K in all three samples. Close to the charge ordering and ferromagnetic transition temperatures the specific heat curves showed peaks superposed to the characteristic response of the lattice oscillations. Below 10 K the specific heat measurements evidenced a Schottky-like anomaly for all samples. However, we could not successfully fit the curves to either a two level nor a distribution of two-level Schottky anomaly. Our results indicated that the peak temperature of the Schottky anomaly was higher in the compounds with narrower conduction band.Comment: submitted to PR

An Origin of CMR: Competing Phases and Disorder-Induced Insulator-to-Metal Transition in Manganites

We theoretically explore the mechanism of the colossal magnetoresistance in manganese oxides by explicitly taking into account the phase competition between the double-exchange ferromagnetism and the charge-ordered insulator. We find that quenched disorder causes a drastic change of the multicritical phase diagram by destroying the charge-ordered state selectively. As a result, there appears a nontrivial phenomenon of the disorder-induced insulator-to-metal transition in the multicritical regime. On the contrary, the disorder induces a highly-insulating state above the transition temperature where charge-ordering fluctuations are much enhanced. The contrasting effects provide an understanding of the mechanism of the colossal magnetoresistance. The obtained scenario is discussed in comparison with other theoretical proposals such as the polaron theory, the Anderson localization, the multicritical-fluctuation scenario, and the percolation scenario.Comment: 16 pages, 7 figures, submitted to Wandlitz Days on Magnetism: Local-Moment Ferromagnets: Unique Properties for Modern Application

Unusual magnetic relaxation behavior in La0.5Ca0.5MnO3 and Nd0.5Sr0.5MnO3

We have carried out a systematic magnetic relaxation study, measured after applying and switching off a 5 T magnetic field to polycrystalline samples of La0.5Ca0.5MnO3 and Nd0.5Sr0.5MnO3. The long time logarithmic relaxation rate (LTLRR), decreased from 10 K to 150 K and increased from 150 K to 195 K in La0.5Ca0.5MnO3. This change in behavior was found to be related to the complete suppression of the antiferromagnetic phase above 150 K and in the presence of a 5 T magnetic field. At 195 K, the magnetization first decreased, and after a few minutes increased slowly as a function of time. Moreover, between 200 K and 245 K, the magnetization increased throughout the measured time span. The change in the slope of the curves, from negative to positive at about 200 K was found to be related to the suppression of antiferromagnetic fluctuations in small magnetic fields. A similar temperature dependence of the LTLRR was found for the Nd0.5Sr0.5MnO3 sample. However, the temperature where the LTLRR reached the minimum in Nd0.5Sr0.5MnO3 was lower than that of La0.5Ca0.5MnO3. This result agrees with the stronger ferromagnetic interactions that exist in Nd0.5Sr0.5MnO3 in comparison to La0.5Ca0.5MnO3. The above measurements suggested that the general temperature dependence of the LTLRR and the underlying physics were mainly independent of the particular charge ordering system considered. All relaxation curves could be fitted using a logarithmic law at long times. This slow relaxation was attributed to the coexistence of ferromagnetic and antiferromagnetic interactions between Mn ions, which produced a distribution of energy barriers.Comment: Accepted to PRB as a regular article, 10 figures, Scheduled Issue: 01 June 200