Search

KV3Sb5 has recently attracted a considerable attention, due to its low temperature superconducting properties, which are heralded by a charge density wave. The apparent presence of a very weak magnetism does not result in long range ordering. We propose a model compatible with a detectable internal magnetic field with no evidence of magnetic long-range order. It invokes higher order terms in the vanadium magnetization density compatible with the presence of a "hidden order" of Dirac (polar) multipoles. The Dirac dipole, known as an anapole or toroidal dipole, is one of a family of electronic multipoles visible in x-ray and magnetic neutron diffraction while undetectable with standard laboratory-based techniques. Two plausible hidden orders are studied with a view to testing in future x-ray and neutron Bragg diffraction experiments whether they are trustworthy. One candidate is magneto-electric and restricted to the linear type, while the other candidate cannot show a magneto-electric effect of any type. The latter hosts a vanadium entity that is both a true scalar and magnetic, and its presence epitomizes an absence of loop currents. Diffraction patterns for the two proposed hidden magnetic orders are distinctly different, fortunately. Corresponding scattering amplitudes for resonant x-ray and neutron Bragg diffraction are calculated with standard chemical and magnetic symmetry tools, and atomic physics.

Critical behavior is very common in many fields of science and a wide variety of many-body systems exhibit emergent critical phenomena. The beauty of critical phase transitions lies in their scale-free properties, such that the temperature dependence of physical parameters of systems differing at the microscopic scale can be described by the same generic power laws. In this work we establish the critical properties of the antiferromagnetic phase transition in artificial square ice, showing that it belongs to the two-dimensional Ising universality class, which extends the applicability of such concepts from atomistic to mesoscopic magnets. Combining soft x-ray resonant magnetic scattering experiments and Monte Carlo simulations, we characterize the transition to the low temperature long range order expected for the artificial square ice system. By measuring the critical scattering, we provide direct quantitative evidence of a continuous magnetic phase transition, obtaining critical exponents which are compatible with those of the two-dimensional Ising universality class. In addition, by varying the blocking temperature relative to the phase transition temperature, we demonstrate its influence on the out-of-equilibrium dynamics due to critical slowing down at the phase transition.

We report the direct observation of a magnetic-feld induced long-wavelength spin spiral modulation in the chiral compound Ba3TaFe3Si2O14. This new spin texture emerges out of a chiral helical ground state, and is hallmarked by the onset of a unique contribution to the bulk electric polarization, the sign of which depends on the crystal chirality. The periodicity of the feld induced modulation, several hundreds of nm depending on the field value, is comparable to the length scales of mesoscopic topological defects such as skyrmions, merons and solitons. The phase transition and observed threshold behavior are consistent with a phenomenology based on the allowed Lifshitz invariants for the chiral symmetry of langasite, which intriguingly contain all the ingredients for the possible realization of topologically stable antiferromagnetic skyrmions.

5d transition metal oxides offer new opportunities to test our understanding of the interplay of correlation effects and spin-orbit interactions in materials in the absence of a single dominant interaction. The subtle balance between solid-state interactions can result in new mechanisms that minimize the interaction energy, and in material properties of potential use for applications. We focus here on the 5d transition metal oxide NaOsO3, a strong candidate for the realization of a magnetically driven transition from a metallic to an insulating state exploiting the so-called Slater mechanism. Experimental results are derived from non-resonant and resonant x-ray single crystal diffraction at the Os L-edges. A change in the crystallographic symmetry does not accompany the metal-insulator transition in the Slater mechanism and, indeed, we find no evidence of such a change in NaOsO3. An equally important experimental observation is the emergence of the (300) Bragg peak in the resonant condition with the onset of magnetic order. The intensity of this space-group forbidden Bragg peak continuously increases with decreasing temperature in line with the square of intensity observed for an allowed magnetic Bragg peak. Our main experimental results, the absence of crystal symmetry breaking and the emergence of a space-group forbidden Bragg peak with developing magnetic order, support the use of the Slater mechanism to interpret the metal-insulator transition in NaOsO3. We successfully describe our experimental results with simulations of the electronic structure and, also, with an atomic model based on the established symmetry of the crystal and magnetic structure., Comment: 6 figures

The control of the electron spin by external means is a key issue for spintronic devices. Using spin- and angle-resolved photoemission spectroscopy (SARPES) with three-dimensional spin detection, we demonstrate operando electrostatic spin manipulation in ferroelectric GeTe and multiferroic Ge1-xMnxTe. We not only demonstrate for the first time electrostatic spin manipulation in Rashba semiconductors due to ferroelectric polarization reversal, but are also able to follow the switching pathway in detail, and show a gain of the Rashba-splitting strength under external fields. In multiferroic Ge1-xMnxTe operando SARPES reveals switching of the perpendicular spin component due to electric field induced magnetization reversal. This provides firm evidence of effective multiferroic coupling which opens up magnetoelectric functionality with a multitude of spin-switching paths in which the magnetic and electric order parameters are coupled through ferroelastic relaxation paths. This work thus provides a new type of magnetoelectric switching entangled with Rashba-Zeeman splitting in a multiferroic system., Comment: 8 pages, 6 figures

X-ray magnetic circular and linear dichroism (XMCD and XMLD) have been used to investigate the Fe magnetic response during the spin reorientation transition (SRT) in TmFeO3. These experiments are complemented with resonant magnetic diffraction experiments at the Tm M5 edge to study simultaneously the induced magnetic order in the Tm 4f shell and the behavior of the Tm orbitals through the SRT. Comparing the Fe XMLD results with neutron diffraction and magnetization measurements on the same sample indicate that the SRT has an enhanced temperature range in the near surface region. This view is supported by the resonant soft x-ray diffraction results at the Tm M5 edge. These find an induced magnetic moment on the Tm sites, which is well-described by a dipolar mean field model originating from the Fe moments. Even though such a model can describe the 4f response in the experiments, it is insufficient to describe the SRT even when considering a change in the 4f anisotropy. Moreover, the results of the Fe XMCD are indicative of a decoupling of spin canting and antiferromagnetic spin rotation in the near surface regime close to the SRT, which remains to be understood., Comment: 28 pages, 12 figures

Chiral multiferroic langasites have attracted attention due to their doubly-chiral magnetic ground state within an enantiomorphic crystal. We report on a detailed resonant soft X-ray diffraction study of the multiferroic Ba$_3$TaFe$_3$Si$_2$O$_{14}$ at the Fe $L_{2,3}$ and oxygen $K$ edges. Below $T_N$ ($\approx27K$) we observe the satellite reflections $(0,0,\tau)$, $(0,0,2\tau)$, $(0,0,3\tau)$ and $(0,0,1-3\tau)$ where $\tau \approx 0.140 \pm 0.001$. The dependence of the scattering intensity on X-ray polarization and azimuthal angle indicate that the odd harmonics are dominated by the out-of-plane ($\mathbf{\hat{c}}$-axis) magnetic dipole while the $(0,0,2\tau)$ originates from the electron density distortions accompanying magnetic order. We observe dissimilar energy dependences of the diffraction intensity of the purely magnetic odd-harmonic satellites at the Fe $L_3$ edge. Utilizing first-principles calculations, we show that this is a consequence of the loss of threefold crystal symmetry in the multiferroic phase.

We performed ultrafast time-resolved near-infrared pump, resonant soft X-ray diffraction probe measurements to investigate the coupling between the photoexcited electronic system and the spin cycloid magnetic order in multiferroic TbMnO3 at low temperatures. We observe melting of the long range antiferromagnetic order at low excitation fluences with a decay time constant of 22.3 +- 1.1 ps, which is much slower than the ~1 ps melting times previously observed in other systems. To explain the data we propose a simple model of the melting process where the pump laser pulse directly excites the electronic system, which then leads to an increase in the effective temperature of the spin system via a slower relaxation mechanism. Despite this apparent increase in the effective spin temperature, we do not observe changes in the wavevector q of the antiferromagnetic spin order that would typically correlate with an increase in temperature under equilibrium conditions. We suggest that this behavior results from the extremely low magnon group velocity that hinders a change in the spin-spiral wavevector on these time scales., Comment: 9 pages, 4 figures

We investigate the structural and magnetic origins of the unusual ultrafast second-harmonicgeneration (SHG) response of femtosecond-laser-excited nickel oxide (NiO) previously attributed to oscillatory reorientation dynamics of the magnetic structure induced by d-d excitations. Using time-resolved x-ray diffraction from the (3/2 3/2 3/2) magnetic planes, we show that changes in the magnitude of the magnetic structure factor following ultrafast optical excitation are limited to $\Delta/$ = 1.5% in the first 30 ps. An extended investigation of the ultrafast SHG response reveals a strong dependence on wavelength as well as characteristic echoes, both of which give evidence for an acoustic origin of the dynamics. We therefore propose an alternative mechanism for the SHG response based on perturbations of the nonlinear susceptibility via optically induced strain in a spatially confined medium. In this model, the two observed oscillation periods can be understood as the times required for an acoustic strain wave to traverse one coherence length of the SHG process in either the collinear or anti-collinear geometries., Comment: 26 pages, 7 figures

Strain is a leading candidate for controlling magnetoelectric coupling in multiferroics. Here, we use x-ray diffraction to study the coupling between magnetic order and structural distortion in epitaxial films of the orthorhombic (o-) perovskite LuMnO$_3$. An antiferromagnetic spin canting in the E-type magnetic structure is shown to be related to the ferroelectrically induced structural distortion and to a change in the magnetic propagation vector. By comparing films of different orientations and thicknesses, these quantities are found to be controlled by b-axis strain. It is shown that compressive strain destabilizes the commensurate E-type structure and reduces its accompanying ferroelectric distortion., Comment: 14 Pages, 4 figures

We present a detailed study on the charge ordering (CO) transition in GdBaCo2O5 system by combining high resolution synchrotron powder/single crystal diffraction with electron paramagnetic resonance (EPR) experiments as a function of temperature. We found a second order structural phase transition at TCO=247 K (Pmmm to Pmma) associated with the onset of long range CO. At Tmin = 1.2TCO, the EPR linewidth rapidly broadens providing evidence of spin fluctuations due to magnetic interactions between Gd3+ ions and antiferromagnetic couplings of Co2+/Co3+ sublattices. This likely indicates that, analogously to manganites, the long-range antiferromagnetic order in GdBaCo2O5 sets in at TCO. Pair distribution function (PDF) analysis of diffraction data revealed signatures of structural inhomogeneities at low temperature. By comparing the average and local bond valences, we found that above TCO the local structure is consistent with a fully random occupation of Co2+ and Co3+ in a 1:1 ratio and with a complete charge ordering below TCO. Below T = 100 K the charge localization is partially melted at the local scale, suggesting a reentrant behavior of CO. This result is supported by the weakening of superstructure reflections and the temperature evolution of EPR linewidth that is consistent with paramagnetic (PM) reentrant behavior reported in the GdBaCo2O5.5 parent compound., Comment: 30 pages, 10 figures

Resonant Bragg diffraction of soft, circularly polarized x-rays has been used to observe directly the temperature dependence of chiral-order melting in a motif of Mn ions in terbium manganate. The underlying mechanism uses the b-axis component of a cycloid, which vanishes outside the polar phase. Melting is witnessed by the first and second harmonics of a cycloid, and we explain why the observed temperature dependence is different in the two harmonics. Our direct observation of melting is supported by a solid foundation of evidence, derived from extensive studies of the azimuthal-angle dependence of intensities with both linear and circular polarization.

Chiral properties of the two phases - collinear motif (below Morin transition temperature, TM=250 K) and canted motif (above TM) - of magnetically ordered hematite ({\alpha}-Fe2O3) have been identified in single crystal resonant x-ray Bragg diffraction, using circular polarized incident x-rays tuned near the iron K-edge. Magneto-electric multipoles, including an anapole, fully characterize the high-temperature canted phase, whereas the low-temperature collinear phase supports both parity-odd and parity-even multipoles that are time-odd. Orbital angular momentum accompanies the collinear motif, while it is conspicuously absent with the canted motif. Intensities have been successfully confronted with analytic expressions derived from an atomic model fully compliant with chemical and magnetic structures. Values of Fe atomic multipoles previously derived from independent experimental data, are shown to be completely trustworthy.

We have used soft x-ray magnetic diffraction at the Fe3+ L2,3 edges to examine to what extent the Dzyaloshinsky-Moriya interaction in Ba3NbFe3Si2O14 influences its low temperature magnetic structure. A modulated component of the moments along the c-axis is present, adding to the previously proposed helical magnetic configuration of co-planar moments in the a,b-plane. This leads to a helical-butterfly structure and suggests that both the multi-axial in-plane and the uniform out-of-plane Dzyaloshinsky-Moriya vectors are relevant. A non zero orbital magnetic signal is also observed at the oxygen K edge, which reflects the surprisingly strong hybridization between iron 3d and oxygen 2p states, given the nominal spherical symmetry of the Fe3+ half filled shell.

We studied the charge-orbital ordering in the superlattice of charge-ordered insulating Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ and ferromagnetic metallic La$_{0.5}$Sr$_{0.5}$MnO$_3$ by resonant soft x-ray diffraction. A temperature-dependent incommensurability is found in the orbital order. In addition, a large hysteresis is observed that is caused by phase competition between insulating charge ordered and metallic ferromagnetic states. No magnetic phase transitions are observed in contrast to bulk, confirming the unique character of the superlattice. The deviation from the commensurate orbital order can be directly related to the decrease of ordered-layer thickness that leads to a decoupling of the orbital-ordered planes along the c axis., Comment: 4 pages, 5 figures

The effect of x-rays on an orbital and charge ordered epitaxial film of a Pr$_{0.5}$Ca$_{0.5}$MnO$_{3}$ is presented. As the film is exposed to x-rays, the antiferromagnetic response increases and concomitantly the conductivity of the film improve. These results are discussed in terms of a persistent x-ray induced doping, leading to a modification of the magnetic structure. This effect allows writing electronic and magnetic domains in the film and represents a novel way of manipulating magnetism., Comment: 5 pages, 5 figures

We investigated the magnetic structure of an orthorhombic YMnO3 thin film by resonant soft x-ray and hard x-ray diffraction. We observed a temperature-dependent incommensurate magnetic reflection below 45 K and a commensurate lattice-distortion reflection below 35 K. These results demonstrate that the ground state is composed of coexisting E-type and cycloidal states. Their different ordering temperatures clarify the origin of the large polarization to be caused by the E-type antiferromagnetic states in the orthorhombic YMnO3 thin film., Comment: 4 pages, 6 figures

We report on the ultrafast dynamics of magnetic order in a single crystal of CuO at a temperature of 207 K in response to strong optical excitation using femtosecond resonant x-ray diffraction. In the experiment, a femtosecond laser pulse induces a sudden, nonequilibrium increase in magnetic disorder. After a short delay ranging from 400 fs to 2 ps, we observe changes in the relative intensity of the magnetic ordering diffraction peaks that indicate a shift from a collinear commensurate phase to a spiral incommensurate phase. These results indicate that the ultimate speed for this antiferromagnetic re-orientation transition in CuO is limited by the long-wavelength magnetic excitation connecting the two phases., Comment: Accepted by Physical Review Letters (Dec. 2, 2011)

Resonant soft x-ray Bragg diffraction at the Dy M$_{4,5}$ edges has been used to study Dy multipoles in the combined magnetic and orbitally ordered phase of DyB$_2$C$_2$. The analysis incorporates both the intra-atomic magnetic and quadrupolar interactions between the 3d core and 4f valence shells. Additionally, we introduce to the formalism the interference of magnetic and nonmagnetic oscillators. This allows a determination of the higher order multipole moments of rank 1 (dipole) to 6 (hexacontatetrapole). The strength of the Dy 4f multipole moments have been estimated at being between 7 and 78 % of the quadrupolar moment., Comment: 11 pages, 2 figures

We present a systematic study of the electronic structure in A-site ordered manganites as function of doping and temperature. The energy dependencies observed with soft x-ray resonant diffraction (SXRD) at the Mn L_{2,3} edges are compared with structural investigations using neutron powder diffraction as well as with cluster calculations. The crystal structures obtained with neutron powder diffraction reflect the various orbital and charge ordered phases and show an increase of the Mn-O-Mn bond angle as function of doping and temperature. Cluster calculations show that the observed spectral changes in SXRD as a function of doping are more pronounced than expected from an increase in bandwitdh due to the increase in Mn-O-Mn bond angle, and are best described by holes that are distributed at the neighbouring oxygen ions. These holes are not directly added to the Mn 3d shell, but centered at the Mn site. In contrast, the spectral changes in SXRD as function of temperature are best described by an increase of magnetic correlations. This demonstrates the strong correlations between orbitals and magnetic moments of the 3d states.

We have investigated the antiferromagnetic insulating phase of the Mott-Hubbard insulator V$_2$O$_3$ by resonant x-ray Bragg diffraction at the vanadium K-edge. Combining the information obtained from azimuthal angle scans, linear incoming polarization scans and by fitting collected data to the scattering amplitude derived from the established chemical I2/a and magnetic space groups we provide evidence of the ordering motif of anapolar moments (which results from parity violation coupling to an electromagnetic field). Experimental data (azimuthal dependence and polarization analysis) collected at space-group forbidden Bragg reflections are successfully accounted within our model in terms of vanadium magnetoelectric multipoles. We demonstrate that resonant x-ray diffraction intensities in all space-group forbidden Bragg reflections of the kind $(hkl)_m$ with odd $h$ are produced by an E1-E2 event. The determined tensorial parameters offer a test for ab-initio calculations in this material, that can lead to a deeper and more quantitative understanding of the physical properties of V$_2$O$_3$.

Geometrical frustration of the Fe ions in LuFe2O4 leads to intricate charge and magnetic order and a strong magnetoelectric coupling. Using resonant x-ray diffraction at the Fe K edge, the anomalous scattering factors of both Fe sites are deduced from the (h/3 k/3 l/2) reflections. The chemical shift between the two types of Fe ions equals 4.0(1) eV corresponding to full charge separation into Fe2+ and Fe3+. Polarization and azimuthal angle dependence of the superlattice reflections demonstrates the absence of anisotropic scattering revealing random orientations of the Fe2+ orbitals characteristic of an orbital glass state., Comment: v2: refined analysis, added supplement, PRL, accepted for publication

We have performed non-resonant x-ray diffraction, resonant soft and hard x-ray magnetic diffraction, soft x-ray absorption and x-ray magnetic circular dichroism measurements to clarify the electronic and magnetic states of the Co3+ ions in GdBaCo2O5.5. Our data are consistent with a 3+ Py Co HS state at the pyramidal sites and a 3+ Oc Co LS state at the octahedral sites. The structural distortion, with a doubling of the a axis (2ap x 2ap x 2ap cell), shows alternating elongations and contractions of the pyramids and indicates that the metal-insulator transition is associated with orbital order in the t2g orbitals of the 3+ Py Co HS state. This distortion corresponds to an alternating ordering of xz and yz orbitals along the a and c axes for the 3+ Py Co . The orbital ordering and pyramidal distortion lead to deformation of the octahedra, but the 3+ Oc Co LS state does not allow an orbital order to occur for the 3+ Oc Co ions. The soft x-ray magnetic diffraction results indicate that the magnetic moments are aligned in the ab plane but are not parallel to the crystallographic a or b axes. The orbital order and the doubling of the magnetic unit cell along the c axis support a non-collinear magnetic structure. The x-ray magnetic circular dichroism data indicate that there is a large orbital magnetic contribution to the total ordered Co moment.

We report the observation of superstructures associated with the oxygen 2p-states in two prototypical manganites using x-ray diffraction at the oxygen K-edge. We determine the nature of the orderings and discuss our picture with respect to novel theoretical models. In the stripe order system Bi0.31 Ca0.69 MnO3, hole-doped O states are found to be orbitally ordered, at the same propagation vector as the Mn orbital ordering, but no evidence is found to support a picture of oxygen charge stripes at this periodicity. In La 7/8 Sr 1/8 MnO3, we observe a 2p charge ordering described by alternating hole-poor and hole-rich MnO planes that is consistent with recent predictions., Comment: 5 pages

Complete polarization analysis applied to resonant x-ray scattering at the Cr K-edge in K2CrO4 shows that incident linearly polarized x-rays can be converted into circularly polarized x-rays by diffraction at the Cr pre-edge (E = 5994 eV). The physical mechanism behind this phenomenon is a subtle interference effect between purely dipole (E1-E1) and purely quadrupole (E2-E2) transitions, leading to a phase shift between the respective scattering amplitudes. This effect may be exploited to disentangle two close-lying resonances that appear as a single peak in a conventional energy scan, in this way allowing to single out and identify the different multipole order parameters involved., Comment: 6 pages, 6 figures

Temperature dependences of a magnetic and an orbital Bragg reflection at the Mn L2 and L3 edges of La0.5Sr1.5MnO4 have been collected. The temperature evolution of the orbital reflection depend strongly on the x-ray energy and reflects the different order parameteres for orbitals and Jahn-Teller distortions. The gradual increase of the orbital order parameter indicates that the orbital order and not the Jahn-Teller distortion drives the metal-insulator transition. Correspondingly, the orbital-orbital (super) exchange interaction dominates over the Jahn-Teller strain-field interaction., Comment: 8 pages, 4 figures

Soft x-ray resonant scattering at the Ni L2,3 edges is used to test models of magnetic and orbital-ordering below the metal-insulator transition in NdNiO3. The large branching ratio of the L3 to L2 intensities of the (1/2,0,1/2) reflection and the observed azimuthal angle and polarization dependence originates from a non collinear magnetic structure. The absence of an orbital signal and the non collinear magnetic structure show that the nickelates are materials for which orbital ordering is absent at the metal-insulator transition., Comment: 10 pages, 4 figures, Physical Review B rapid communication, to be published

Resonant soft x-ray Bragg diffraction at the Tb M4,5 edges and non resonant Bragg diffraction have been used to investigate orbitals in TbB2C2. The Tb 4f quadrupole moments are ordered in zero field below T_N and show a ferroquadrupolar alignment dictated by the antiferromagnetic order. With increasing applied field along [110] the Tb 4f magnetic dipole moments rotate in a gradual manner toward the field. The quadrupole moment is rigidly coupled to the magnetic moment and follows this field-induced rotation. The quadrupolar pair interaction is found to depend on the specific orientation of the orbitals as predicted theoretically and can be manipulated with an applied magnetic field., Comment: 4 pages, 4 figures. Updated title, abstract, introduction and references

Resonant soft x-ray Bragg diffraction at the Dy M4,5 edges has been exploited to study Dy multipole motifs in DyB2C2. Our results are explained introducing the intra-atomic quadrupolar interaction between the core 3d and valence 4f shell. This allows us to determine for the first time higher order multipole moments of dysprosium $4f$ electrons and to draw their precise charge density. The Dy hexadecapole and hexacontatetrapole moment have been estimated at -20% and +30% of the quadrupolar moment, respectively. No evidence for the lock-in of the orbitals at T_N has been observed, in contrast to earlier suggestions. The multipolar interaction and the structural transition cooperate along c but they compete in the basal plane explaining the canted structure along [110]., Comment: 4 pages, 3 figures