Structural response to O*-O' and magnetic transitions in orthorhombic perovskites

We present a temperature dependent single crystal x-ray diffraction study of twinned orthorhombic perovskites La1-xCaxMnO3, for x=0.16 and x=0.25. These data show the evolution of the crystal structure from the ferromagnetic insulating state to the ferromagnetic metallic state. The data are modelled in space group Pnma with twin relations based on a distribution of the b axis over three perpendicular cubic axes. The twin model allows full structure determination in the presence of up to six twin fractions using the single crystal x-ray diffraction data.Comment: 13 pages, including 13 figures and 2 table

Commensurate-Incommensurate transition in the melting process of the orbital ordering in Pr0.5Ca0.5MnO3: neutron diffraction study

The melting process of the orbital order in Pr0.5Ca0.5MnO3 single crystal has been studied in detail as a function of temperature by neutron diffraction. It is demonstrated that a commensurate-incommensurate (C-IC) transition of the orbital ordering takes place in a bulk sample, being consistent with the electron diffraction studies. The lattice structure and the transport properties go through drastic changes in the IC orbital ordering phase below the charge/orbital ordering temperature Tco/oo, indicating that the anomalies are intimately related to the partial disordering of the orbital order, unlike the consensus that it is related to the charge disordering process. For the same T range, partial disorder of the orbital ordering turns on the ferromagnetic spin fluctuations which were observed in a previous neutron scattering study.Comment: 5 pages, 2 figures, REVTeX, to be published in Phys. Rev.

Ferromagnetic Polarons in La0.5Ca0.5MnO3 and La0.33Ca0.67MnO3

Unrestricted Hartree-Fock calculations on La0.5Ca0.5MnO3 and La0.33Ca0.67MnO3 in the full magnetic unit cell show that the magnetic ground states of these compounds consist of 'ferromagnetic molecules' or polarons ordered in herring-bone patterns. Each polaron consists of either three or five Mn ions separated by O- ions with a magnetic moment opposed to those of the Mn ions. Ferromagnetic coupling within the polarons is strong while coupling between them is relatively weak. Magnetic moments on the Mn ions range between 3.8 and 3.9 Bohr magnetons in La0.5Ca0.5MnO3 and moments on the O- ions are -0.7 Bohr magnetons. Each polaron has a net magnetic moment of 7.0 Bohr magnetons, in good agreement with recently reported magnetisation measurements from electron microscopy. The polaronic nature of the electronic structure reported here is obviously related to the Zener polaron model recently proposed for Pr0.6Ca0.4MnO3 on the basis of neutron scattering data.Comment: 4 pages 5 figure

Effect of band-filling and structural distortions on the Curie temperature of Fe-Mo double perovkites

By means of high resolution neutron powder diffraction at low temperature we have characterized the structural details of $\rm La_{x}Sr_{2-x}FeMoO_6$ ($0\leq {\rm x}\leq 0.5$) and $\rm Ca_{x}Sr_{2-x}FeMoO_6$ ($0\leq {\rm x}\leq 0.6$) series of compounds. This study reveals a similar variation of the mean bond-angle \FeOMo in both series. In contrast, the mean bond-distance \FeMoO\ increases with La but not with Ca substitution. Both series also present a different evolution of the Curie temperature ($T_C$), which raises in the La series and slightly decreases in the Ca one. We thus conclude that the enhancement of $T_C$ in the La series is due to the electron filling of the conduction band and a concomitant rising of the density of states at the Fermi level.Comment: Revtex, 4 Journal pages, 2 figures, 1 tabl

Giant positive magnetoresistance in metallic VOx thin films

We report on giant positive magnetoresistance effect observed in VOx thin films, epitaxially grown on SrTiO3 substrate. The MR effect depends strongly on temperature and oxygen content and is anisotropic. At low temperatures its magnitude reaches 70% in a magnetic field of 5 T. Strong electron-electron interactions in the presence of strong disorder may qualitatively explain the results. An alternative explanation, related to a possible magnetic instability, is also discussed.Comment: 4 pages, 5 figures included in the text, references update

Cooling rate dependence of the antiferromagnetic domain structure of a single crystalline charge ordered manganite

The low temperature phase of single crystals of Nd$_{0.5}$Ca$_{0.5}$MnO$_3$ and Gd$_{0.5}$Ca$_{0.5}$MnO$_3$ manganites is investigated by squid magnetometry. Nd$_{0.5}$Ca$_{0.5}$MnO$_3$ undergoes a charge-ordering transition at $T_{CO}$=245K, and a long range CE-type antiferromagnetic state is established at $T_N$=145K. The dc-magnetization shows a cooling rate dependence below $T_N$, associated with a weak spontaneous moment. The associated excess magnetization is related to uncompensated spins in the CE-type antiferromagnetic structure, and to the presence in this state of fully orbital ordered regions separated by orbital domain walls. The observed cooling rate dependence is interpreted to be a consequence of the rearrangement of the orbital domain state induced by the large structural changes occurring upon cooling.Comment: REVTeX4; 7 pages, 4 figures. Revised 2001/12/0

Selective Spin-State Switch and Metal-Insulator Transition in \boldmath GdBaCo2O5.5\rm GdBaCo_2O_{5.5}

Ultra-high resolution synchrotron diffraction data for $\rm GdBaCo_2O_{5.5}$ throw new light on the metal-insulator transition of Co$^{3+}$ Ba-cobaltites. An anomalous expansion of CoO$_6$ octahedra is observed at the phase transition on heating, while CoO$_5$ pyramids show the normal shrinking at the closing of the gap. The insulator-to-metal transition is attributed to a sudden excitation of some electrons in the octahedra ($t_{2g}^6$ state) into the Co $e_g$ band (final $t_{2g}^4e_g^2$ state). The $t_{2g}^5e_g^1$ state in the pyramids does not change and the structural study also rules out a $d_{3x^2-r^2}/d_{3y^2-r^2}$ orbital ordering at $T_{MI}$.Comment: Phys. Rev. B (to appear

Orbital Ordering in Paramagnetic LaMnO3 and KCuF3

{\it Ab-initio} studies of the stability of orbital ordering, its coupling to magnetic structure and its possible origins (electron-phonon and/or electron-electron interactions) are reported for two perovskite systems, LaMnO$_3$ and KCuF$_3$. We present a new Average Spin State (ASS) calculational scheme that allowed us to treat a paramagnetic state. Using this scheme, we succesfully described the experimental magnetic/orbital phase diagram of both LaMnO$_3$ and KCuF$_3$ in crystal structures when the Jahn-Teller distortions are neglected. Hence, we conclude that the orbital ordering in both compounds is purely electronic in origin.Comment: 10 pages, 5 figure

Anisotropic Superexchange for nearest and next nearest coppers in chain, ladder and lamellar cuprates

We present a detailed calculation of the magnetic couplings between nearest-neighbor and next-nearest-neighbor coppers in the edge-sharing geometry, ubiquitous in many cuprates. In this geometry, the interaction between nearest neighbor coppers is mediated via two oxygens, and the Cu-O-Cu angle is close to 90 degrees. The derivation is based on a perturbation expansion of a general Hubbard Hamiltonian, and produces numerical estimates for the various magnetic energies. In particular we find the dependence of the anisotropy energies on the angular deviation away from the 90 degrees geometry of the Cu-O-Cu bonds. Our results are required for the correct analysis of the magnetic structure of various chain, ladder and lamellar cuprates.Comment: 13 pages, Latex, 7 figure

Ab initio investigation of VOSeO3, a spin gap system with coupled spin dimers

Motivated by an early experimental study of VOSeO3, which suggested that it is a quasi-2D system of weakly coupled spin dimers with a small spin gap, we have investigated the electronic structure of this material via density-functional calculations. These ab initio results indicate that the system is better thought of as an alternating spin-1/2 chain with moderate interchain interactions, an analog of (VO)2P2O7. The potential interest of this system for studies in high magnetic field given the presumably small value of the spin gap is emphasized.Comment: 4 pages, 5 figure