Direct determination of the spin structure of Nd2_2Ir2_2O7_7 by means of neutron diffraction

We report on the spin structure of the pyrochlore iridate Nd$_2$Ir$_2$O$_7$ that could be directly determined by means of powder neutron diffraction. Our magnetic structure refinement unravels a so-called all-in/all-out magnetic structure that appears in both, the Nd and the Ir sublattice. The ordered magnetic moments at 1.8 K amount to 0.34(1) $\mu_\mathrm{B}$/Ir$^{4+}$ and 1.27(1) $\mu_\mathrm{B}$/Nd$^{3+}$. The Nd$^{3+}$ moment size at 1.8 K is smaller than that expected for the Nd$^{3+}$ ground state doublet. On the other hand, the size of the ordered moments of the Ir$^{4+}$ ions at 1.8 K agrees very well with the value expected for a $J_\mathrm{eff}$ = 1/2 state based on the presence of strong spin-orbit coupling in this system. Finally, our measurements reveal a parallel alignment of the Nd$^{3+}$ moments with the net moment of its six nearest neighboring Ir$^{4+}$ ions.Comment: http://journals.aps.org/prb/pdf/10.1103/PhysRevB.94.16110

Hour-glass magnetic spectrum in a stripe-less insulating transition metal oxide

An hour-glass shaped magnetic excitation spectrum appears to be an universal characteristic of the high-temperature superconducting cuprates. Fluctuating charge stripes or alternative band structure approaches are able to explain the origin of these spectra. Recently, an hour- glass spectrum has been observed in an insulating cobaltate, thus, favouring the charge stripe scenario. Here we show that neither charge stripes nor band structure effects are responsible for the hour-glass dispersion in a cobaltate within the checkerboard charge ordered regime of La2-xSrxCoO4. The search for charge stripe ordering reflections yields no evidence for charge stripes in La1.6Sr0.4CoO4 which is supported by our phonon studies. With the observation of an hour-glass-shaped excitation spectrum in this stripe-less insulating cobaltate, we provide experimental evidence that the hour-glass spectrum is neither necessarily connected to charge stripes nor to band structure effects, but instead, probably intimately coupled to frustration and arising chiral or non-collinear magnetic correlations

Multiferroicity in the frustrated spinel cuprate GeCu2_2O4_4

Different from other magnetically frustrated spinel systems, GeCu$_{2}$O$_{4}$ is a strongly tetragonal distorted spinel cuprate in which edge-sharing CuO$_{2}$ ribbons are running along alternating directions perpendicular to the $c$-axis. Here, GeCu$_{2}$O$_{4}$ samples of high quality were prepared via high pressure synthesis (at 4 GPa) and the corresponding magnetic and dielectric properties were investigated. For the first time, we observed a ferroelectric polarization emerging at T$_{N}$ $\sim$ 33~K. Although the ferroelectric polarization is weak in GeCu$_{2}$O$_{4}$ ($P$ $\sim$ 0.2$\mu$C/m$^{2}$), the existence of spin-induced multiferroicity provides a strong constraint on the possible ground state magnetic structures and/or the corresponding theoretical models of multiferroicity for GeCu$_{2}$O$_{4}$.Comment: https://journals.aps.org/prmaterials/abstract/10.1103/PhysRevMaterials.2.04140

Verwey transition in Fe3_{3}O4_{4} thin films: Influence of oxygen stoichiometry and substrate-induced microstructure

We have carried out a systematic experimental investigation to address the question why thin films of Fe$_3$O$_4$ (magnetite) generally have a very broad Verwey transition with lower transition temperatures as compared to the bulk. We observed using x-ray photoelectron spectroscopy, x-ray diffraction and resistivity measurements that the Verwey transition in thin films is drastically influenced not only by the oxygen stoichiometry but especially also by the substrate-induced microstructure. In particular, we found (1) that the transition temperature, the resistivity jump, and the conductivity gap of fully stoichiometric films greatly depends on the domain size, which increases gradually with increasing film thickness, (2) that the broadness of the transition scales with the width of the domain size distribution, and (3) that the hysteresis width is affected strongly by the presence of antiphase boundaries. Films grown on MgO (001) substrates showed the highest and sharpest transitions, with a 200 nm film having a T$_V$ of 122K, which is close to the bulk value. Films grown on substrates with large lattice constant mismatch revealed very broad transitions, and yet, all films show a transition with a hysteresis behavior, indicating that the transition is still first order rather than higher order.Comment: 9 pages, 12 figure

Magnetostrictive Neel ordering of the spin-5/2 ladder compound BaMn2O3: distortion-induced lifting of geometrical frustration

The crystal structure and the magnetism of BaMn$_2$O$_3$ have been studied by thermodynamic and by diffraction techniques using large single crystals and powders. BaMn$_2$O$_3$ is a realization of a $S = 5/2$ spin ladder as the magnetic interaction is dominant along 180$^\circ$ Mn-O-Mn bonds forming the legs and the rungs of a ladder. The temperature dependence of the magnetic susceptibility exhibits well-defined maxima for all directions proving the low-dimensional magnetic character in BaMn$_2$O$_3$. The susceptibility and powder neutron diffraction data, however, show that BaMn$_2$O$_3$ exhibits a transition to antiferromagnetic order at 184 K, in spite of a full frustration of the nearest-neighbor inter-ladder coupling in the orthorhombic high-temperature phase. This frustration is lifted by a remarkably strong monoclinic distortion which accompanies the magnetic transition.Comment: 9 pages, 8 figures, 2 tables; in V1 fig. 2 was included twice and fig. 4 was missing; this has been corrected in V

Magnetically induced Ferroelectricity in Bi2_2CuO4_4

The tetragonal copper oxide Bi$_2$CuO$_4$ has an unusual crystal structure with a three-dimensional network of well separated CuO$_4$ plaquettes. This material was recently predicted to host electronic excitations with an unconventional spectrum and the spin structure of its magnetically ordered state appearing at T$_N$ $\sim$43 K remains controversial. Here we present the results of detailed studies of specific heat, magnetic and dielectric properties of Bi$_2$CuO$_4$ single crystals grown by the floating zone technique, combined with the polarized neutron scattering and high-resolution X-ray measurements. Our polarized neutron scattering data show Cu spins are parallel to the $ab$ plane. Below the onset of the long range antiferromagnetic ordering we observe an electric polarization induced by an applied magnetic field, which indicates inversion symmetry breaking by the ordered state of Cu spins. For the magnetic field applied perpendicular to the tetragonal axis, the spin-induced ferroelectricity is explained in terms of the linear magnetoelectric effect that occurs in a metastable magnetic state. A relatively small electric polarization induced by the field parallel to the tetragonal axis may indicate a more complex magnetic ordering in Bi$_2$CuO$_4$

Control of multiferroic domains by external electric fields in TbMnO3

The control of multiferroic domains through external electric fields has been studied by dielectric measurements and by polarized neutron diffraction on single-crystalline TbMnO$_3$. Full hysteresis cycles were recorded by varying an external field of the order of several kV/mm and by recording the chiral magnetic scattering as well as the charge in a sample capacitor. Both methods yield comparable coercive fields that increase upon cooling.Comment: 12 pages, 6 figure

Distinct magnetic ground states of R2R_2ZnIrO6_6 (RR = La and Nd) determined by neutron powder diffraction

Double perovskite iridates $A_2$ZnIrO$_6$ ($A$ = alkaline or lanthanide) show complex magnetic behaviors ranging from weak ferromagnetism to successive antiferromagnetic transitions. Here we report the static ($dc$) and dynamic ($ac$) magnetic susceptibility, and neutron powder diffraction measurements for $A$ = La and Nd compounds to elucidate the magnetic ground state. Below 10~K, the $A$ = La compound is best described as canted iridium moments in an antiferromagnet arrangement with a propagation vector \textbf{k} = 0 and a net ferromagnetic component along the $c$-axis. On the other hand, Nd$_2$ZnIrO$_6$ is described well as an antiferromagnet with a propagation vector \textbf{k} = (1/2~1/2~0) below $T_\mathrm{N} \sim$ 17 K. Scattering from both the Nd and Ir magnetic sublattices were required to describe the data and both were found to lie almost completely within the $ab$-plane. $Dc$ susceptibility revealed a bifurcation between the zero-field-cooled and field-cooled curves below $\sim$13 K in Nd$_2$ZnIrO$_6$. A glassy state was ruled out by $ac$ susceptibility but detailed magnetic isotherms revealed the opening of the loop below 13~K. These results suggest a delicate balance exists between the Dzyaloshinskii-Moriya, crystal field schemes, and $d$-$f$ interaction in this series of compounds.Comment: 6 pages, 5 figures. To be published in PR

Intricacies of the Co3+^{3+} spin state in Sr2_2Co0.5_{0.5}Ir0.5_{0.5}O4_4: an x-ray absorption and magnetic circular dichroism study

We report on a combined soft x-ray absorption and magnetic circular dichroism (XMCD) study at the Co-$L_{3,2}$ on the hybrid 3$d$/5$d$ solid state oxide Sr$_2$Co$_{0.5}$Ir$_{0.5}$O$_4$ with the K$_2$NiF$_4$ structure. Our data indicate unambiguously a pure high spin state $(S=2)$ for the Co$^{3+}$ (3$d^6$) ions with a significant unquenched orbital moment $L_z/2S_z=0.25$ despite the sizeable elongation of the CoO$_6$ octahedra. Using quantitative model calculations based on parameters consistent with our spectra, we have investigated the stability of this high spin state with respect to the competing low spin and intermediate spin states.Comment: 7 pages, 4 figure

Magnetoelastic coupling in RETiO3 (RE = La, Nd, Sm, Gd, Y)

A detailed analysis of the crystal structure in RETiO3 with RE = La, Nd, Sm, Gd, and Y reveals an intrinsic coupling between orbital degrees of freedom and the lattice which cannot be fully attributed to the structural deformation arising from bond-length mismatch. The TiO6 octahedra in this series are all irregular with the shape of the distortion depending on the RE ionic radius. These octahedron distortions vary more strongly with temperature than the tilt and rotation angles. Around the Ti magnetic ordering all compounds exhibit strong anomalies in the thermal-expansion coefficients, these anomalies exhibit opposite signs for the antiferromagnetic and ferromagnetic compounds. Furthermore the strongest effects are observed in the materials close to the magnetic cross-over from antiferromagnetic to ferromagnetic order