Magnetically-induced electric polarization in an organo-metallic magnet

The coupling between magnetic order and ferroelectricity has been under intense investigation in a wide range of transition-metal oxides. The strongest coupling is obtained in so-called magnetically-induced multiferroics where ferroelectricity arises directly from magnetic order that breaks inversion symmetry. However, it has been difficult to find non-oxide based materials in which these effects occur. Here we present a study of copper dimethyl sulfoxide dichloride (CDC), an organo-metallic quantum magnet containing $S = 1/2$ Cu spins, in which electric polarization arises from non-collinear magnetic order. We show that the electric polarization can be switched in a stunning hysteretic fashion. Because the magnetic order in CDC is mediated by large organic molecules, our study shows that magnetoelectric interactions can exist in this important class of materials, opening the road to designing magnetoelectrics and multiferroics using large molecules as building blocks. Further, we demonstrate that CDC undergoes a magnetoelectric quantum phase transition where both ferroelectric and magnetic order emerge simultaneously as a function of magnetic field at very low temperatures

Magnetic properties of GdT2T_2Zn20_{20} (T = Fe, Co) investigated by X-ray diffraction and spectroscopy

We investigate the magnetic and electronic properties of the Gd$T_2$Zn$_{20}$ ($T$ = Fe and Co) compounds using X-ray resonant magnetic scattering (XRMS), X-ray absorption near-edge structure (XANES) and X-ray magnetic circular dichroism (XMCD) techniques. The XRMS measurements reveal that the GdCo$_2$Zn$_{20}$ compound has a commensurate antiferromagnetic spin structure with a magnetic propagation vector $\vec{\tau}$ = $(\frac{1}{2},\frac{1}{2},\frac{1}{2})$ below the N\'eel temperature ($T_N \sim$ 5.7 K). Only the Gd ions carry a magnetic moment forming an antiferromagnetic structure with magnetic representation $\Gamma_6$. For the ferromagnetic GdFe$_2$Zn$_{20}$ compound, an extensive investigation was performed at low temperature and under magnetic field using XANES and XMCD techniques. A strong XMCD signal of about 12.5 $\%$ and 9.7 $\%$ is observed below the Curie temperature ($T_C \sim$ 85 K) at the Gd-$L_2$ and $L_3$ edges, respectively. In addition, a small magnetic signal of about 0.06 $\%$ of the jump is recorded at the Zn $K$-edge suggesting that the Zn 4$p$ states are spin polarized by the Gd 5$d$ extended orbitals

High-magnetic field lattice length changes in URu2Si2

We report high magnetic field (up to 45 T) c-axis thermal expansion and magnetostriction experiments on URu2Si2 single crystals. The sample length change associated with the transition to the hidden order phase becomes increasingly discontinous as the magnetic field is raised above 25 T. The re-entrant ordered phase III is clearly observed in both the thermal expansion and magnetostriction above 36 T, in good agreement with previous results. The sample length is also discontinuous at the boundaries of this phase, mainly at the upper boundary. A change in the sign of the coefficient of thermal-expansion is observed at the metamagnetic transition (B_M = 38 T) which is likely related to the existence of a quantum critical end point.Comment: 5 pages, 4 figures, to be published in PR

Origin of the high Seebeck coefficient of the misfit [Ca2_2CoO3_3]0.62_{0.62}[CoO2_2] cobaltate from site-specific valency and spin-state determinations

Layered misfit cobaltate [Ca$_2$CoO$_3$]$_{0.62}$[CoO$_2$], which emerged as an important thermoelectric material~[A. C. Masset et al. Phys. Rev. B, 62, 166 (2000)], has been explored extensively in the last decade for the exact mechanism behind its high Seebeck coefficient. Its complex crystal and electronic structures have inhibited consensus among such investigations. This situation has arisen mainly due to difficulties in accurate identification of the chemical state, spin state, and site symmetries in its two subsystems (rocksalt [Ca$_2$CoO$_3$] and triangular [CoO$_2$]). By employing resonant photoemission spectroscopy and x-ray absorption spectroscopy along with charge transfer multiplet simulations (at the Co ions), we have successfully identified the site symmetries, valencies and spin states of the Co in both layers. Our site-symmetry observations explain the experimental value of the high Seebeck coefficient and also confirm that the carriers hop within the rocksalt layer, which is in contrast to earlier reports where hopping within triangular CoO$_2$ layer has been held responsible for the large Seebeck coefficient.Comment: 5 pages, 4 figures and 1 supplementary with 3 figure

Magnetic Properties Of Gdt2zn20 (t=fe, Co) Investigated By X-ray Diffraction And Spectroscopy

We investigate the magnetic and electronic properties of the GdT2Zn20 (T=Fe and Co) compounds using x-ray resonant magnetic scattering (XRMS), x-ray absorption near-edge structure (XANES), and x-ray magnetic circular dichroism (XMCD). The XRMS measurements reveal that GdCo2Zn20 has a commensurate antiferromagnetic spin structure with a magnetic propagation vector τ - =(12,12,12) below the Néel temperature (TN∼5.7 K). Only the Gd ions carry a magnetic moment forming an antiferromagnetic structure with magnetic representation Γ6. For the ferromagnetic GdFe2Zn20 compound, an extensive investigation was performed at low temperature and under magnetic field using XANES and XMCD. A strong XMCD signal of about 12.5% and 9.7% is observed below the Curie temperature (TC∼85K) at the Gd L2 and L3 edges, respectively. In addition, a small magnetic signal of about 0.06% of the jump is recorded at the Zn K edge, suggesting that the Zn 4p states are spin polarized by the Gd 5d extended orbitals. © 2016 American Physical Society.93

Magnetic and orbital correlations in multiferroic CaMn7_7O12_{12} probed by x-ray resonant elastic scattering

The quadruple perovskite CaMn$_7$O$_{12}$ is a topical multiferroic, in which the hierarchy of electronic correlations driving structural distortions, modulated magnetism, and orbital order is not well known and may vary with temperature. x-ray resonant elastic scattering (XRES) provides a momentum-resolved tool to study these phenomena, even in very small single crystals, with valuable information encoded in its polarization- and energy-dependence. We present an application of this technique to CaMn$_7$O$_{12}$. By polarization analysis, it is possible to distinguish superstructure reflections associated with magnetic order and orbital order. Given the high momentum resolution, we resolve a previously unknown splitting of an orbital order superstructure peak, associated with a distinct \textit{locked-in} phase at low temperatures. A second set of orbital order superstructure peaks can then be interpreted as a second-harmonic orbital signal. Surprisingly, the intensities of the first- and second-harmonic orbital signal show disparate temperature and polarization dependence. This orbital re-ordering may be driven by an exchange mechanism, that becomes dominant over the Jahn-Teller instability at low temperature.Comment: 6 pages, 4 figures and 1 supplementary with 3 figure

Ferromagnetic Kitaev interaction and the origin of large magnetic anisotropy in α\alpha-RuCl3_3

$\alpha$-RuCl$_3$ is drawing much attention as a promising candidate Kitaev quantum spin liquid. However, despite intensive research efforts, controversy remains about the form of the basic interactions governing the physics of this material. Even the sign of the Kitaev interaction (the bond-dependent anisotropic interaction responsible for Kitaev physics) is still under debate, with conflicting results from theoretical and experimental studies. The significance of the symmetric off-diagonal exchange interaction (referred to as the $\Gamma$ term) is another contentious question. Here, we present resonant elastic x-ray scattering data that provides unambiguous experimental constraints to the two leading terms in the magnetic interaction Hamiltonian. We show that the Kitaev interaction ($K$) is ferromagnetic, and that the $\Gamma$ term is antiferromagnetic and comparable in size to the Kitaev interaction. Our findings also provide a natural explanation for the large anisotropy of the magnetic susceptibility in $\alpha$-RuCl$_3$ as arising from the large $\Gamma$ term. We therefore provide a crucial foundation for understanding the interactions underpinning the exotic magnetic behaviours observed in $\alpha$-RuCl$_3$.Comment: 5 pages, two-column, 3 figure

Single-crystal X-ray diffraction and resonant X-ray magnetic scattering at helium-3 temperatures in high magnetic fields at beamline P09 at PETRA III

The resonant scattering and diffraction beamline P09 at PETRA III at DESY is equipped with a 14 T vertical field split-pair magnet. A helium-3 refrigerator is available that can be fitted inside the magnet\u27s variable-temperature insert. Here the results of a series of experiments aimed at determining the beam conditions permitting operations with the He-3 insert are presented. By measuring the tetragonal-to-orthorhombic phase transition occurring at 2.1 K in the Jahn-Teller compound TmVO4, it is found that the photon flux at P09 must be attenuated down to 1.5 × 109 photons s-1 for the sample to remain at temperatures below 800 mK. Despite such a reduction of the incident flux and the subsequent use of a Cu(111) analyzer, the resonant X-ray magnetic scattering signal at the Tm LIII absorption edge associated with the spin-density wave in TmNi2B2C below 1.5 K is intense enough to permit a complete study in magnetic field and at sub-Kelvin temperatures to be carried out

Spin waves and spin-state transitions in a ruthenate high-temperature antiferromagnet

Ruthenium compounds play prominent roles in materials research ranging from oxide electronics to catalysis, and serve as a platform for fundamental concepts such as spin-triplet superconductivity, Kitaev spin-liquids, and solid-state analogues of the Higgs mode in particle physics. However, basic questions about the electronic structure of ruthenates remain unanswered, because several key parameters (including the Hund's-rule, spin-orbit, and exchange interactions) are comparable in magnitude, and their interplay is poorly understood - partly due to difficulties in synthesizing sizable single crystals for spectroscopic experiments. Here we introduce a resonant inelastic x-ray scattering (RIXS) technique capable of probing collective modes in microcrystals of $4d$-electron materials. We present a comprehensive set of data on spin waves and spin-state transitions in the honeycomb antiferromagnet SrRu$_{2}$O$_{6}$, which possesses an unusually high N\'eel temperature. The new RIXS method provides fresh insight into the unconventional magnetism of SrRu$_{2}$O$_{6}$, and enables momentum-resolved spectroscopy of a large class of $4d$ transition-metal compounds.Comment: The original submitted version of the published manuscript. https://www.nature.com/articles/s41563-019-0327-