Pressure-induced colossal piezoresistance effect and the collapse of the polaronic state in the bilayer manganite (La(0.4)Pr(0.6))(1.2)Sr(1.8)Mn2O7

We have investigated the effect of hydrostatic pressure as a function of temperature on the resistivity of a single crystal of the bilayer manganite (La(0.4)Pr(0.6))(1.2)Sr(1.8)Mn(2)O(7). Whereas a strong insulating behaviour is observed at all temperatures at ambient pressure, a clear transition into a metallic-like behaviour is induced when the sample is subjected to a pressure (P) of ~1.0 GPa at T < 70 K. A huge negative piezoresistance ~10(6) in the low temperature region at moderate pressures is observed. When the pressure is increased further (5.5 GPa), the high temperature polaronic state disappears and a metallic behaviour is observed. The insulator to metal transition temperature exponentially increases with pressure and the distinct peak in the resistivity that is observed at 1.0 GPa almost vanishes for P > 7.0 GPa. A modification in the orbital occupation of the e(g) electron between 3d(x(2)-y(2)) and 3d(z(2)-r(2)) states, as proposed earlier, leading to a ferromagnetic double-exchange phenomenon, can qualitatively account for our data.     

Charge/orbital ordering structure of Pr(1-x)Ca(x)MnO(3)(x = 3/8) examined by low-temperature transmission electron microscopy

The structural phase transition of Pr(1-x)Ca(x)MnO(3)(x = 3/8) was investigated by means of low-temperature transmission electron microscopy. Superlattice reflection spots with a modulation wave vector q(1) = (0,1/2,0) appeared below 230 K, indicating formation of the d(3x(2-r(2))/d(3y(2)-r(2)) type of charge/orbital ordering. Below 150 K, a new series of superlattice reflection spots with a modulation wave vector q(2) = (1/4,1/4,1/2) appeared, suggesting an additional ordering of excess 1/8 Mn(3+), necessary due to the deviation of x from 1/2, with the occupation of the d(3z(2-r(2)) type of e(g) orbital.     

Hidden magnetic configuration in epitaxial La(1-x) Sr(x) MnO3 films

We present an unreported magnetic configuration in epitaxial La(1-x) Sr(x) MnO3 (x ～ 0.3) (LSMO) films grown on strontium titanate (STO). X-ray magnetic circular dichroism indicates that the remanent magnetic state of thick LSMO films is opposite to the direction of the applied magnetic field. Spectroscopic and scattering measurements reveal that the average Mn valence varies from mixed Mn(3+)/Mn(4+) to an enriched Mn3+ region near the STO interface, resulting in a compressive lattice along the a, b axis and a possible electronic reconstruction in the Mn e(g) orbital (d(3)z(2)-r(2). This reconstruction may provide a mechanism for coupling the Mn3+ moments antiferromagnetically along the surface normal direction, and in turn may lead to the observed reversed magnetic configuration.     

Crystal-field level inversion in lightly Mn-doped Sr3Ru2O7

Sr3(Ru(1-x)Mnx)2O7, in which 4d-Ru is substituted by the more localized 3d-Mn, is studied by x-ray dichroism and spin-resolved density functional theory. We find that Mn impurities do not exhibit the same 4+ valence of Ru, but act as 3+ acceptors; the extra eg electron occupies the in-plane 3d(x2-y2) orbital instead of the expected out-of-plane 3d(3z2-r2). We propose that the 3d-4d interplay, via the ligand oxygen orbitals, is responsible for this crystal-field level inversion and the material's transition to an antiferromagnetic, possibly orbitally ordered, low-temperature state.     

Pressure tuning of magnetic interactions in layered (La0.6Nd0.4)1. 2Sr1.8Mn2O7 manganite

The effect of pressure of up to 9 GPa on the magnetic and structural properties of layered (La0.6Nd0.4)1.2Sr1.8Mn2O7 manganite has been investigated. Pressure shifts the Mn atoms from the center of each bilayer towards the adjacent bilayer. The observed shift of the Mn atoms involves mainly a charge redistribution within the d(3z(2)-r(2)) axial orbital. The decrease in the interbilayer spacing and the shift of the Mn atoms away from the center of each bilayer result in increased magnetic and electronic coupling between the adjacent bilayers along the c axis.     

Evidence of orbital reconstruction at interfaces in ultrathin La0.67Sr0.33MnO3 films

Linear dichroism (LD) in x-ray absorption, diffraction, transport, and magnetization measurements on thin La(0.7)Sr(0.3)MnO(3) films grown on different substrates, allow identification of a peculiar interface effect, related just to the presence of the interface. We report the LD signature of preferential 3d-e(g)(3z(2)-r(2)) occupation at the interface, suppressing the double exchange mechanism. This surface orbital reconstruction is opposite to that favored by residual strain and is independent of dipolar fields, the chemical nature of the substrate and the presence of capping layers.     

Orbital nature of ferromagnetic magnons in manganites

Magnon excitation in a ferromagnetic state of Sm(0.55)Sr(0.45)MnO(3) located on the verge of the metal-insulator transition has been studied in terms of the neutron scattering experiment. The anomalous magnon dispersion with the zone-boundary softening is well described by the Heisenberg model with extended exchange coupling constants J(s). In particular the fourth neighbor coupling J(4) is as large as 0.6 times the nearest neighbor one J(1). Theoretical analysis based on the local density approximation + Hubbard U band calculation reveals that this one-dimensional exchange path is due to the (3z(2)-r(2))-type orbital correlation, in sharp contrast to previous proposals.     

Steplike lattice deformation of single crystalline (La0.4Pr0.6)1.2Sr1.8Mn2O7 bilayered manganite

We report a steplike lattice transformation of single crystalline (La0.4Pr0.6)1.2Sr1.8Mn2O7 bilayered manganite accompanied by both magnetization and magnetoresistive jumps, and examine the ultrasharp nature of the field-induced first-order transition from a paramagnetic insulator to a ferromagnetic metal phase accompanied by a huge decrease in resistance. Our findings support that the abrupt magnetostriction is closely related to an orbital frustration existing in the inhomogeneous paramagnetic insulating phase rather than a martensitic scenario between competing two phases.     

Quasi-one-dimensional magnetism driven by unusual orbital ordering in CuSb2O6

Essentially all undoped cuprates exhibit a quasiplanar, fourfold Cu-O coordination responsible for the magnetically active antibonding 3d(x(2)-y(2)) like state. Here, we present an electronic structure study for CuSb(2)O(6) that reveals, in contrast, a half-filled 3d(3z(2)-r(2)) orbital. This hitherto unobserved ground state originates from a competition of in- and out-of-plaquette orbitals where the strong Coulomb repulsion drives the surprising and unique orbital ordering. This, in turn, gives rise to an unexpected quasi-one-dimensional magnetic behavior. Our results provide a consistent explanation of recent thermodynamical and neutron diffraction measurements.     

O1s and Mn2p NEXAFS on single-layered La1-xSr1+xMnO4: crystal field effect versus orbital coupling mechanism

O1s and Mn2p near-edge X-ray absorption spectroscopy on La_1-xSr_1+xMnO₄ (0 ≤x ≤0.5) single crystals shows that Sr doping does not only provide holes to the system but also induces a continuous transfer of electrons from out-of-plane d_3z2-r2 to in-plane d_3x2-r2/d_3y2-r2 orbitals. Furthermore, a non-vanishing electron occupation of in-plane d_x2-y2 and out-of-plane d_3z2-r2 orbitals is observed up to relatively high doping contents. These findings demonstrate that the energy difference between all these orbital types has to be very small and manifest that the orbital degree of freedom is determined not just by crystal field effects but also by orbital coupling. Moreover, the doping-dependent transfer of spectral weight observed in the current data identifies La_1-xSr_1+xMnO₄ as a charge-transfer insulator.     

Independent freezing of charge and spin dynamics in La1.5Sr0.5CoO4

We present elastic and quasielastic neutron scattering measurements characterizing peculiar short-range charge-orbital and spin order in the layered perovskite material La1.5Sr0.5CoO4. We find that below T(c) approximately 750 K holes introduced by Sr doping lose mobility and enter a statically ordered charge glass phase with loosely correlated checkerboard arrangement of empty and occupied d(3z(2)-r(2)) orbitals ( Co3+ and Co2+). The dynamics of the resultant mixed spin system is governed by the anisotropic nature of the crystal-field Hamiltonian and the peculiar exchange pattern produced by the orbital order. It undergoes a spin freezing transition at a much lower temperature, T(s) less, similar30 K.     

Surface states of cobalt nanoislands on Cu111

The electronic structure of thin Co nanoislands on Cu(111) has been investigated below and above the Fermi level (E(F)) by scanning tunneling spectroscopy at low temperature. Two surface related electronic states are found: a strong localized peak 0.31 eV below E(F) and a mainly unoccupied dispersive state, giving rise to quantum interference patterns of standing electron waves on the Co surface. Ab initio calculations reveal that the electronic states are spin polarized, originating from d3(z(2)-r(2))-minority and sp-majority bands, respectively.     

Electronic and Magnetic States of Pr and Mn in the Pr<Subscript>1–<Emphasis Type="Italic">x</Emphasis></Subscript>Sr<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>MnO<Subscript>3</Subscript> Films Studied by XANES and XMCD Spectroscopy

The spectral dependences of X-ray absorption near-edge spectroscopy (XANES) and X-ray magnetic circular dichroism (XMCD) and the field dependences of XMCD near the K edge of Mn and the L_2,3 edges of Pr in the Pr_0.8Sr_0.2MnO₃ and Pr_0.6Sr_0.4MnO₃ films at T = 90 K are studied. The spectral dependences point to a mixed valence state of Mn and Pr in the films. It is found that, as compared to XANES, XMCD is more sensitive to the valence state of Pr⁴⁺. The field dependences of XMCD point to ferromagnetic behavior of Mn ions and the Van Vleck paramagnetism of Pr ions, which makes a significant contribution to the total magnetization of the films. It is shown that as the Sr concentration increases, the XMCD intensity at the K edge of Mn increases, which indicates a growth of the total magnetic moment of the film due to an increase in the 4p–3d hybridization.     

Field-induced ferromagnetic metallic state in the bilayer manganite (La0.4Pr0.6)1.2Sr1.8Mn2O7, probed by neutron scattering

The bilayer manganite La1.2Sr1.8Mn2O7 exhibits a phase transition from a paramagnetic insulating (PI) to a ferromagnetic metallic (FM) state with a colossal magnetoresistance (CMR) effect. Upon 60% Pr substitution, magnetic order and PI to FM transition are suppressed. Application of a moderate magnetic field restores an FM state with a CMR effect. Neutron scattering by a single crystal of (La0.4Pr0.6)1.2Sr1.8Mn2O7, under a magnetic field of 5 T, has revealed a long-range and homogeneous ferromagnetic order. In the PI phase, under zero field, correlated lattice polarons have been detected. At 28 K, under 5 T, the spin wave dispersion curve determines an in-plane isotropic spin wave stiffness constant of 146 meV A(2). So the magnetic field not only generates a homogeneous ferromagnetic ground state, but also restores a magnetic coupling characteristic of FM CMR manganites.     

Observation of magnetic ripple and nanowidth domains in a layered ferromagnet

We investigated ferromagnetic domain structures on nanometer to micrometer scale for single crystals of a layered ferromagnet, La(2-2x)Sr(1+2x)Mn2O7 (0.32 < or = x < or = 0.40), as functions of x and temperature by means of Lorentz electron microscopy. We have succeeded in observing the evolution of magnetic ripple structure, dynamically, related to a spin reorientation transition where the magnetization direction switches between parallel and perpendicular to the layers. Our high-resolution magnetic domain imaging revealed that the ripple state is characterized by the evolution of magnetic nanowidth domains.     

Effects of R-site compositions on the meta-magnetic behavior of Tb_(1-x)Pr_x(Fe_(0.4)Co_(0.6))_(1.88)C_(0.05)(x=0, 0.8, and 1)

We investigate the low-temperature magnetic properties of intermetallic compounds Tb1-xPrx(Fe0.4Co0.6)1.88C0.05(x = 0, 0.8, and 1) by detailed magnetization measurements. Obvious temperature- and field-induced irreversibilities suggest the coexistence of multiple magnetic phases. Sharp magnetization jumps across the antiferromagnetic to ferromagnetic transition are observed only in the Pr-containing samples, indicating that the behavior of the avalanche-like growth of ferromagnetic clusters is mainly related to the light lanthanide Pr ions. In addition, the time relaxation, field sweep rate, and cooling field dependence of magnetization jumps in the sample with x = 1 are consistent with those in the martensitic scenario.     

Electronic confinement and ordering instabilities in colossal magnetoresistive bilayer manganites

We present angle-resolved photoemission studies of (La{1-z}Pr{z}){2-2x}Sr{1+2x}Mn{2}O{7} with x=0.4 and z=0.1, 0.2, and 0.4 along with density functional theory calculations and x-ray scattering data. Our results show that the bilayer splitting in the ferromagnetic metallic phase of these materials is small, if not completely absent. The charge carriers are therefore confined to a single MnO{2} layer, which in turn results in a strongly nested Fermi surface. In addition to this, the spectral function also displays clear signatures of an electronic ordering instability well below the Fermi level. The increase of the corresponding interaction strength with z and its magnitude of ～400 meV make the coupling to a bare phonon highly unlikely. Instead we conclude that fluctuating order, involving electronic and lattice degrees of freedom, causes the observed renormalization of the spectral features.     

Anomalous spin-density distribution on oxygen and Ru in Ca(1.5)Sr(0.5)RuO(4): polarized neutron diffraction study

By means of polarized neutron diffraction in a magnetic field of 7.0 T at 1.6 K an anomalously large magnetization density is observed on the in-plane oxygen in Ca(1.5)Sr(0.5)RuO(4). Field-induced moments of different ions are determined by refinement on the flipping ratios, yielding micro(Ru)=0.346(11)micro(B), micro(O1)=0.076(6)micro(B), and micro(O2)=0.009(6)micro(B). The moment on the oxygen arises from the strong hybridization between the Ru-4d and O-2p orbitals. The maximum entropy magnetization density reconstruction reveals a strongly anisotropic density at the Ru site, consistent with the distribution of the xy (t(2g) band) d orbitals.     

Current oscillation and low-field colossal magnetoresistance effect in phase-separated manganites

Current-induced switching from a metallic to an insulating state is observed in phase-separated states of (La(1-y)Pr(y))0.7Ca0.3MnO3 (y=0.7) and Nd(0.5)Ca(0.5)Mn(1-z)Cr(z)O3 (z=0.03) crystals. The application of magnetic fields to this current-induced insulating state causes a pronounced low-field negative magnetoresistance effect [rho(H)/rho(0)=10(-3) at H=1 kOe]. The application of a constant voltage also causes the breakdown of the Ohmic relation above a threshold voltage. At voltages higher than this threshold value, oscillations in currents are observed. This oscillation is well reproduced by a simple model of local switching of a percolative conduction path.     

Field-induced magnetic transition in a Cu-Mn spin-glass alloy

The time-independent magnetization of a Cu-Mn alloy (9 at% Mn) as an isothermal function of field is found to describe an S-shaped curve indicative of a field-induced transition. The critical field for the transition decreases to zero as the temperature is raised to that of the susceptibility cusp.