Spin canted magnetism, decoupling of charge and spin ordering in NdNiO3_3

We report detailed magnetization measurements on the perovskite oxide NdNiO$_3$. This system has a first order metal-insulator (M-I) transition at about 200 K which is associated with charge ordering. There is also a concurrent paramagnetic to antiferromagnetic spin ordering transition in the system. We show that the antiferromagnetic state of the nickel sublattice is spin canted. We also show that the concurrency of the charge ordering and spin ordering transitions is seen only while warming up the system from low temperature. The transitions are not concurrent while cooling the system through the M-I transition temperature. This is explained based on the fact that the charge ordering transition is first order while the spin ordering transition is continuous. In the magnetically ordered state the system exhibits ZFC-FC irreversibilities, as well as history-dependent magnetization and aging. Our analysis rules out the possibility of spin-glass or superparamagnetism and suggests that the irreversibilities originate from magnetocrystalline anisotropy and domain wall pinning.Comment: 8 pages, 7 figure

Spin-orbit induced mixed-spin ground state in RRNiO3_3 perovskites probed by XAS: new insight into the metal to insulator transition

We report on a Ni L$_{2,3}$ edges x-ray absorption spectroscopy (XAS) study in $R$NiO$_3$ perovskites. These compounds exhibit a metal to insulator ($MI$) transition as temperature decreases. The L$_{3}$ edge presents a clear splitting in the insulating state, associated to a less hybridized ground state. Using charge transfer multiplet calculations, we establish the importance of the crystal field and 3d spin-orbit coupling to create a mixed-spin ground state. We explain the $MI$ transition in $R$NiO$_3$ perovskites in terms of modifications in the Ni$^{3+}$ crystal field splitting that induces a spin transition from an essentially low-spin (LS) to a mixed-spin state.Comment: 4 pages, 4 figures, accepted as PRB - Rapid Comm. Dez. 200

Unprecedented magnetoresistance in Cd-substituted Tl2Mn2O7 pyrochlores

3 pages, 3 figures.Moderate pressure techniques (P = 20 kbar) have been used to prepare Tl2–xCdxMn2O7 (0x0.4) pyrochlore-like materials. The x = 0.2 compound has been characterized by neutron powder diffraction, magnetic, magnetotransport, and Hall measurements. This material is ferromagnetic below TC = 110 K. Both electrical resistance and magnetoresistance (MR) are enhanced with respect to stoichiometric Tl2Mn2O7, due to the drastic reduction in the number of carriers (electrons) induced by hole doping. MR(0.5 T) is higher than 106% at 120 K, and MR(9 T) is 30% at room temperature. We show that hole doped derivatives of Tl2Mn2O7 are promising candidates in which to search for large bulk magnetoresistance.The author are grateful for the financial support of CICyT (Project Nos. PB97-1181 and MAT99-1045).Peer reviewe

Infinite Layer LaNiO(2): Ni(1+)is not Cu(2+)

The Ni ion in LaNiO$_2$ has the same formal ionic configuration $3d^9$ as does Cu in isostructural CaCuO$_2$, but it is reported to be nonmagnetic and probably metallic whereas CaCuO$_2$ is a magnetic insulator. From ab initio calculations we trace its individualistic behavior to (1) reduced $3d-2p$ mixing due to an increase of the separation of site energies ($\epsilon_d - \epsilon_p$) of at least 2 eV, and (2) important Ni $3d(3z^2-r^2)$ mixing with La $5d(3z^2-r^2)$ states that leads to Fermi surface pockets of La $5d$ character that hole-dope the Ni 3d band.Correlation effects do not appear to be large in LaNiO$_2$. However, ad hoc increase of the intraatomic repulsion on the Ni site (using the LDA+U method) is found to lead to a novel correlated state: (i) the transition metal $d(x^2-y^2)$ and $d(3z^2-r^2)$ states undergo consecutive Mott transitions, (ii) their moments are antialigned leading (ideally) to a "singlet" ion in which there are two polarized orbitals, and (iii) mixing of the upper Hubbard $3d(3z^2-r^2)$ band with the La $5d(xy)$ states leaves considerable transition metal 3d character in a band pinned to the Fermi level. The magnetic configuration is more indicative of a Ni$^{2+}$ ion in this limit, although the actual charge changes little with U.Comment: 7 pages, 8 figure

Electronic structure, local magnetism, and spin-orbit effects of Ir(IV)-, Ir(V)-, and Ir(VI)-based compounds

Element- and orbital-selective x-ray absorption and magnetic circular dichroism measurements are carried out to probe the electronic structure and magnetism of Ir 5d electronic states in double perovskite Sr2MIrO6 (M=Mg, Ca, Sc, Ti, Ni, Fe, Zn, In) and La2NiIrO6 compounds. All the studied systems present a significant influence of spin-orbit interactions in the electronic ground state. In addition, we find that the Ir 5d local magnetic moment shows different character depending on the oxidation state despite the net magnetization being similar for all the compounds. Ir carries an orbital contribution comparable to the spin contribution for Ir4+ (5d5) and Ir5+ (5d4) oxides, whereas the orbital contribution is quenched for Ir6+ (5d3) samples. Incorporation of a magnetic 3d atom allows getting insight into the magnetic coupling between 5d and 3d transition metals. Together with previous susceptibility and neutron diffraction measurements, the results indicate that Ir carries a significant local magnetic moment even in samples without a 3d metal. The size of the (small) net magnetization of these compounds is a result of predominant antiferromagnetic interactions between local moments coupled with structural details of each perovskite structure.This work was partially supported by the Spanish MINECO Projects No. MAT2014-54425-R and No. MAT2013-41099-R and by the Comunidad de Madrid Project No. S2009/PPQ-1551. M. A. Laguna-Marco acknowledges CSIC and European Social Fund for a JAE-Doc contract. Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357.Peer Reviewe

Reflectividad, transmisión y actividad fotoinducida del RNiO3 (r=Pr,Sm) en el infrarrojo

Con el fin de esclarecer el mecanismo responsable de la transición metal-aislador que experimentan RNiO₃, (R - Pr, Sm) a Tm.a ∼135K y ∼403K respectivamente, se ha estudiado con espectroscopia infrarroja la evolución con la temperatura de los espectros de reflectividad, transmisión y la actividad fotoinducida. Los espectros de reflectividad se ajustaron por medio de una simulación de la función dieléctrica mediante un modelo clásico de osciladores de Lorentz amortiguados a los que se agregó un término de Drude para describir el comportamiento del plasma. La conductividad óptica experimental así determinada ha sido analizada empleando la teoría de pequeños polarones de Heese v Reik. El análisis de los espectros de reflectividad y el excelente acuerdo hallado entre la teoría de pequeños polarones y los resultados experimentales nos ha permitido verificar la intensidad de la interacción electrón-fonón y así confirmar la participación determinante de fonones en las propiedades de transporte de RNi0₃ (R=Pr, Sm). De esta manera, la transición metal-aislador esta directamente relacionada con la localización a TM.A de electrones auto atrapados en entornos polarónicos.Centro de Química Inorgánic

First order transition and phase separation in pyrochlores with colossal-magnetoresistance

Tl$_{2}$Mn$_{2}$O$_{7}$ pyrochlores present colossal magnetoresistance (CMR) around the long range ferromagnetic ordering temperature (T$_{C}$). The character of this magnetic phase transition has been determined to be first order, by purely magnetic methods, in contrast to the second order character previously reported by Zhao et al. (Phys. Rev. Lett. 83, 219 (1999)). The highest CMR effect, as in Tl$_{1.8}$Cd$_{0.2}$Mn$_{2}$O$_{7}$, corresponds to a stronger first order character. This character implies a second type of magnetic interaction, besides the direct superexchange between the Mn$^{4+}$ ions, as well as a phase coexistence. A model is proposed, with a complete Hamiltonian (including superexchange and an indirect interaction), which reproduce the observed phenomenology.Comment: 6 pages. Figures include

On the fraction of dark matter in charged massive particles (CHAMPs)

From various cosmological, astrophysical and terrestrial requirements, we derive conservative upper bounds on the present-day fraction of the mass of the Galactic dark matter (DM) halo in charged massive particles (CHAMPs). If dark matter particles are neutral but decay lately into CHAMPs, the lack of detection of heavy hydrogen in sea water and the vertical pressure equilibrium in the Galactic disc turn out to put the most stringent bounds. Adopting very conservative assumptions about the recoiling velocity of CHAMPs in the decay and on the decay energy deposited in baryonic gas, we find that the lifetime for decaying neutral DM must be > (0.9-3.4)x 10^3 Gyr. Even assuming the gyroradii of CHAMPs in the Galactic magnetic field are too small for halo CHAMPs to reach Earth, the present-day fraction of the mass of the Galactic halo in CHAMPs should be < (0.4-1.4)x 10^{-2}. We show that redistributing the DM through the coupling between CHAMPs and the ubiquitous magnetic fields cannot be a solution to the cuspy halo problem in dwarf galaxies.Comment: 21 pages, 2 figures. To appear in JCA

Raman phonons as a probe of disorder, fluctuations and local structure in doped and undoped orthorhombic and rhombohedral manganites

We present a rationalization of the Raman spectra of orthorhombic and rhombohedral, stoichiometric and doped, manganese perovskites. In particular we study RMnO3 (R= La, Pr, Nd, Tb, Ho, Er, Y and Ca) and the different phases of Ca or Sr doped RMnO3 compounds as well as cation deficient RMnO3. The spectra of manganites can be understood as combinations of two kinds of spectra corresponding to two structural configurations of MnO6 octahedra and independently of the average structure obtained by diffraction techniques. The main peaks of compounds with regular MnO6 octahedra, as CaMnO3, highly Ca doped LaMnO3 or the metallic phases of Ca or Sr doped LaMnO3, are bending and tilt MnO6 octahedra modes which correlate to R-O(1) bonds and Mn-O-Mn angles respectively. In low and optimally doped manganites, the intensity and width of the broad bands are related to the amplitude of the dynamic fluctuations produced by polaron hopping in the paramagnetic insulating regime. The activation energy, which is proportional to the polaron binding energy, is the measure of this amplitude. This study permits to detect and confirm the coexistence, in several compounds, of a paramagnetic matrix with lattice polaron together with regions without dynamic or static octahedron distortions, identical to the ferromagnetic metallic phase. We show that Raman spectroscopy is an excellent tool to obtain information on the local structure of the different micro or macro-phases present simultaneously in many manganites.Comment: Submitted to PR