Magnetic monopole density and antiferromagnetic domain control in spin-ice iridates.

Magnetically frustrated systems provide fertile ground for complex behaviour, including unconventional ground states with emergent symmetries, topological properties, and exotic excitations. A canonical example is the emergence of magnetic-charge-carrying quasiparticles in spin-ice compounds. Despite extensive work, a reliable experimental indicator of the density of these magnetic monopoles is yet to be found. Using measurements on single crystals of Ho2Ir2O7 combined with dipolar Monte Carlo simulations, we show that the isothermal magnetoresistance is highly sensitive to the monopole density. Moreover, we uncover an unexpected and strong coupling between the monopoles on the holmium sublattice and the antiferromagnetically ordered iridium ions. These results pave the way towards a quantitative experimental measure of monopole density and demonstrate the ability to control antiferromagnetic domain walls using a uniform external magnetic field, a key goal in the design of next-generation spintronic devices.

Charge Condensation and Lattice Coupling Drives Stripe Formation in Nickelates.

Revealing the predominant driving force behind symmetry breaking in correlated materials is sometimes a formidable task due to the intertwined nature of different degrees of freedom. This is the case for La_{2-x}Sr_{x}NiO_{4+δ}, in which coupled incommensurate charge and spin stripes form at low temperatures. Here, we use resonant x-ray photon correlation spectroscopy to study the temporal stability and domain memory of the charge and spin stripes in La_{2-x}Sr_{x}NiO_{4+δ}. Although spin stripes are more spatially correlated, charge stripes maintain a better temporal stability against temperature change. More intriguingly, charge order shows robust domain memory with thermal cycling up to 250 K, far above the ordering temperature. These results demonstrate the pinning of charge stripes to the lattice and that charge condensation is the predominant factor in the formation of stripe orders in nickelates.

Selective probing of magnetic order on Tb and Ir sites in stuffed Tb2Ir2O7  using resonant x-ray scattering.

We study the magnetic structure of the 'stuffed' (Tb-rich) pyrochlore iridate Tb2+x Ir2-x O7-y  (x ∼ 0.18), using resonant elastic x-ray scattering (REXS). In order to disentangle contributions from Tb and Ir magnetic sublattices, experiments were performed at the Ir L 3 and Tb M 5 edges, which provide selective sensitivity to Ir 5d and Tb 4f  magnetic moments, respectively. At the Ir L 3 edge, we found the onset of long-range [Formula: see text] magnetic order below [Formula: see text] K, consistent with the expected signal of all-in all-out (AIAO) magnetic order. Using a single-ion model to calculate REXS cross-sections, we estimate an ordered magnetic moment of [Formula: see text] at 5 K. At the Tb M 5 edge, long-range [Formula: see text] magnetic order appeared below ∼[Formula: see text] K, also consistent with an AIAO magnetic structure on the Tb site. Additional insight into the magnetism of the Tb sublattice is gleaned from measurements at the M 5 edge in applied magnetic fields up to 6 T, which is found to completely suppress the Tb AIAO magnetic order. In zero applied field, the observed gradual onset of the Tb sublattice magnetisation with temperature suggests that it is induced by the magnetic order on the Ir site. The persistence of AIAO magnetic order, despite the greatly reduced ordering temperature and moment size compared to stoichiometric Tb2Ir2O7, for which [Formula: see text] K and [Formula: see text], indicates that stuffing could be a viable means of tuning the strength of electronic correlations, thereby potentially offering a new strategy to achieve topologically non-trivial band crossings in pyrochlore iridates.

Role of defects in determining the magnetic ground state of ytterbium titanate.

Pyrochlore systems are ideally suited to the exploration of geometrical frustration in three dimensions, and their rich phenomenology encompasses topological order and fractional excitations. Classical spin ices provide the first context in which it is possible to control emergent magnetic monopoles, and anisotropic exchange leads to even richer behaviour associated with large quantum fluctuations. Whether the magnetic ground state of Yb2Ti2O7 is a quantum spin liquid or a ferromagnetic phase induced by a Higgs transition appears to be sample dependent. Here we have determined the role of structural defects on the magnetic ground state via the diffuse scattering of neutrons. We find that oxygen vacancies stabilise the spin liquid phase and the stuffing of Ti sites by Yb suppresses it. Samples in which the oxygen vacancies have been eliminated by annealing in oxygen exhibit a transition to a ferromagnetic phase, and this is the true magnetic ground state.

Doping Dependence of Collective Spin and Orbital Excitations in the Spin-1 Quantum Antiferromagnet La_{2-x}Sr_{x}NiO_{4} Observed by X Rays.

We report the first empirical demonstration that resonant inelastic x-ray scattering (RIXS) is sensitive to collective magnetic excitations in S=1 systems by probing the Ni L_{3} edge of La_{2-x}Sr_{x}NiO_{4} (x=0, 0.33, 0.45). The magnetic excitation peak is asymmetric, indicating the presence of single and multi-spin-flip excitations. As the hole doping level is increased, the zone boundary magnon energy is suppressed at a much larger rate than that in hole doped cuprates. Based on the analysis of the orbital and charge excitations observed by RIXS, we argue that this difference is related to the orbital character of the doped holes in these two families. This work establishes RIXS as a probe of fundamental magnetic interactions in nickelates opening the way towards studies of heterostructures and ultrafast pump-probe experiments.

All-in-all-Out Magnetic Order and Propagating Spin Waves in Sm_{2}Ir_{2}O_{7}.

Using resonant magnetic x-ray scattering we address the unresolved nature of the magnetic ground state and the low-energy effective Hamiltonian of Sm_{2}Ir_{2}O_{7}, a prototypical pyrochlore iridate with a finite temperature metal-insulator transition. Through a combination of elastic and inelastic measurements, we show that the magnetic ground state is an all-in-all-out (AIAO) antiferromagnet. The magnon dispersion indicates significant electronic correlations and can be well described by a minimal Hamiltonian that includes Heisenberg exchange [J=27.3(6) meV] and Dzyaloshinskii-Moriya interactions [D=4.9(3) meV], which provides a consistent description of the magnetic order and excitations. In establishing that Sm_{2}Ir_{2}O_{7} has the requisite inversion symmetry preserving AIAO magnetic ground state, our results support the notion that pyrochlore iridates may host correlated Weyl semimetals.

Direct evidence for charge stripes in a layered cobalt oxide.

Recent experiments indicate that static stripe-like charge order is generic to the hole-doped copper oxide superconductors and competes with superconductivity. Here we show that a similar type of charge order is present in La5/3Sr1/3CoO4, an insulating analogue of the copper oxide superconductors containing cobalt in place of copper. The stripe phase we have detected is accompanied by short-range, quasi-one-dimensional, antiferromagnetic order, and provides a natural explanation for the distinctive hourglass shape of the magnetic spectrum previously observed in neutron-scattering measurements of La2-xSrxCoO4 and many hole-doped copper oxide superconductors. The results establish a solid empirical basis for theories of the hourglass spectrum built on short-range, quasi-static, stripe correlations.

Anisotropic local modification of crystal field levels in Pr-based pyrochlores: a muon-induced effect modeled using density functional theory.

Although muon spin relaxation is commonly used to probe local magnetic order, spin freezing, and spin dynamics, we identify an experimental situation in which the measured response is dominated by an effect resulting from the muon-induced local distortion rather than the intrinsic behavior of the host compound. We demonstrate this effect in some quantum spin ice candidate materials Pr(2)B(2)O(7) (B=Sn, Zr, Hf), where we detect a static distribution of magnetic moments that appears to grow on cooling. Using density functional theory we show how this effect can be explained via a hyperfine enhancement arising from a splitting of the non-Kramers doublet ground states on Pr ions close to the muon, which itself causes a highly anisotropic distortion field. We provide a quantitative relationship between this effect and the measured temperature dependence of the muon relaxation and discuss the relevance of these observations to muon experiments in other magnetic materials.

Mechanism of spin crossover in LaCoO3 resolved by shape magnetostriction in pulsed magnetic fields.

In the scientific description of unconventional transport properties of oxides (spin-dependent transport, superconductivity etc.), the spin-state degree of freedom plays a fundamental role. Because of this, temperature- or magnetic field-induced spin-state transitions are in the focus of solid-state physics. Cobaltites, e.g. LaCoO3, are prominent examples showing these spin transitions. However, the microscopic nature of the spontaneous spin crossover in LaCoO3 is still controversial. Here we report magnetostriction measurements on LaCoO3 in magnetic fields up to 70 T to study the sharp, field-induced transition at Hc ≈ 60 T. Measurements of both longitudinal and transversal magnetostriction allow us to separate magnetovolume and magnetodistortive changes. We find a large increase in volume, but only a very small increase in tetragonal distortion at Hc. The results, supported by electronic energy calculations by the configuration interaction cluster method, provide compelling evidence that above Hc LaCoO3 adopts a correlated low spin/high spin state.

High-temperature electromagnons in the magnetically induced multiferroic cupric oxide driven by intersublattice exchange.

Magnetically induced ferroelectric multiferroics present an exciting new paradigm in the design of multifunctional materials, by intimately coupling magnetic and polar order. Magnetoelectricity creates a novel quasiparticle excitation--the electromagnon--at terahertz frequencies, with spectral signatures that unveil important spin interactions. To date, electromagnons have been discovered at low temperature (<70 K) and predominantly in rare-earth compounds such as RMnO3. Here we demonstrate using terahertz time-domain spectroscopy that intersublattice exchange in the improper multiferroic cupric oxide (CuO) creates electromagnons at substantially elevated temperatures (213-230 K). Dynamic magnetoelectric coupling can therefore be achieved in materials, such as CuO, that exhibit minimal static cross-coupling. The electromagnon strength and energy track the static polarization, highlighting the importance of the underlying cycloidal spin structure. Polarized neutron scattering and terahertz spectroscopy identify a magnon in the antiferromagnetic ground state, with a temperature dependence that suggests a significant role for biquadratic exchange.

Restoration of the third law in spin ice thin films.

A characteristic feature of spin ice is its apparent violation of the third law of thermodynamics. This leads to a number of interesting properties including the emergence of an effective vacuum for magnetic monopoles and their currents - magnetricity. Here we add a new dimension to the experimental study of spin ice by fabricating thin epitaxial films of Dy2Ti2O7, varying between 5 and 60 monolayers on an inert substrate. The films show the distinctive characteristics of spin ice at temperatures >2 K, but at lower temperature we find evidence of a zero entropy state. This restoration of the third law in spin ice thin films is consistent with a predicted strain-induced ordering of a very unusual type, previously discussed for analogous electrical systems. Our results show how the physics of frustrated pyrochlore magnets such as spin ice may be significantly modified in thin-film samples.

Absence of strong magnetic fluctuations in FeP-based systems LaFePO and Sr2ScO3FeP.

We report neutron inelastic scattering measurements on polycrystalline LaFePO and Sr2ScO3FeP, two members of the iron phosphide families of superconductors. No evidence is found for any magnetic fluctuations in the spectrum of either material in the energy and wavevector ranges probed. Special attention is paid to the wavevector at which spin-density-wave-like fluctuations are seen in other iron-based superconductors. We estimate that the magnetic signal, if present, is at least a factor of four (Sr2ScO3FeP) or seven (LaFePO) smaller than in the related iron arsenide and chalcogenide superconductors. These results suggest that magnetic fluctuations are not as influential on the electronic properties of the iron phosphide systems as they are in other iron-based superconductors.

Suppression of thermal conductivity by rattling modes in thermoelectric sodium cobaltate.

The need for both high electrical conductivity and low thermal conductivity creates a design conflict for thermoelectric systems, leading to the consideration of materials with complicated crystal structures. Rattling of ions in cages results in low thermal conductivity, but understanding the mechanism through studies of the phonon dispersion using momentum-resolved spectroscopy is made difficult by the complexity of the unit cells. We have performed inelastic X-ray and neutron scattering experiments that are in remarkable agreement with our first-principles density-functional calculations of the phonon dispersion for thermoelectric Na(0.8)CoO2, which has a large-period superstructure. We have directly observed an Einstein-like rattling mode at low energy, involving large anharmonic displacements of the sodium ions inside multi-vacancy clusters. These rattling modes suppress the thermal conductivity by a factor of six compared with vacancy-free NaCoO2. Our results will guide the design of the next generation of materials for applications in solid-state refrigerators and power recovery.

The Jeff = 1/2 insulator Sr3Ir2O7 studied by means of angle-resolved photoemission spectroscopy.

The low-energy electronic structure of the J(eff) = 1/2 spin-orbit insulator Sr3Ir2O7 has been studied by means of angle-resolved photoemission spectroscopy. A comparison of the results for bilayer Sr3Ir2O7 with available literature data for the related single-layer compound Sr2IrO4 reveals qualitative similarities and similar J(eff) = 1/2 bandwidths for the two materials, but also pronounced differences in the distribution of the spectral weight. In particular, photoemission from J(eff) = 1/2 the states appears to be suppressed. Yet, it is found that the Sr3Ir2O7 data are in overall better agreement with band-structure calculations than the data for Sr2IrO4.

On the magnetic structure of Sr3Ir2O7: an x-ray resonant scattering study.

This report presents azimuthal dependent and polarization dependent x-ray resonant magnetic scattering at the Ir L(3) edge for the bilayered iridate compound Sr(3)Ir(2)O(7). The two magnetic wave vectors, k1 = (1/2, 1/2, 0) and k2 = (1/2, -1/2, 0), result in domains of two symmetry-related G-type antiferromagnetic structures, denoted A and B, respectively. These domains are approximately 0.02 mm(2) and are independent of the thermal history. An understanding of this key aspect of the magnetism is necessary for an overall picture of the magnetic behaviour in this compound. The azimuthal and polarization dependence of the magnetic reflections, relating to both magnetic wavevectors, show that the Ir magnetic moments in the bilayer compound are oriented along the c axis. This contrasts with single layer Sr(2)IrO(4) where the moments are confined to the ab plane.

Femtosecond dynamics of the collinear-to-spiral antiferromagnetic phase transition in CuO.

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 reorientation transition in CuO is limited by the long-wavelength magnetic excitation connecting the two phases.

Ground state in a half-doped manganite distinguished by neutron spectroscopy.

We have measured the spin-wave spectrum of the half-doped bilayer manganite Pr(Ca,Sr)(2)Mn(2)O(7) in its spin, charge, and orbital ordered phase. The measurements, which extend throughout the Brillouin zone and cover the entire one-magnon spectrum, are compared critically with spin-wave calculations for different models of the electronic ground state. The data are described very well by the Goodenough model, which has weakly interacting ferromagnetic zig-zag chains in the CE-type arrangement. A model that allows ferromagnetic dimers to form within the zigzags is inconsistent with the data. The analysis conclusively rules out the strongly bound dimer (Zener polaron) model.

Cu3Nb2O8: a multiferroic with chiral coupling to the crystal structure.

By combining bulk properties, neutron diffraction, and nonresonant x-ray diffraction measurements, we demonstrate that the new multiferroic Cu(3)Nb(2)O(8) becomes polar simultaneously with the appearance of generalized helicoidal magnetic ordering. The electrical polarization is oriented perpendicularly to the common plane of rotation of the spins-an observation that cannot be reconciled with the conventional theory developed for cycloidal multiferroics. Our results are consistent with coupling between a macroscopic structural rotation, which is allowed in the paramagnetic group, and magnetically induced structural chirality.

Femtoscale magnetically induced lattice distortions in multiferroic TbMnO3.

Magneto-electric multiferroics exemplified by TbMnO(3) possess both magnetic and ferroelectric long-range order. The magnetic order is mostly understood, whereas the nature of the ferroelectricity has remained more elusive. Competing models proposed to explain the ferroelectricity are associated respectively with charge transfer and ionic displacements. Exploiting the magneto-electric coupling, we used an electric field to produce a single magnetic domain state, and a magnetic field to induce ionic displacements. Under these conditions, interference between charge and magnetic x-ray scattering arose, encoding the amplitude and phase of the displacements. When combined with a theoretical analysis, our data allow us to resolve the ionic displacements at the femtoscale, and show that such displacements make a substantial contribution to the zero-field ferroelectric moment.

Photoinduced melting of antiferromagnetic order in La(0.5)Sr(1.5)MnO4 measured using ultrafast resonant soft x-ray diffraction.

We used ultrafast resonant soft x-ray diffraction to probe the picosecond dynamics of spin and orbital order in La(0.5)Sr(1.5)MnO(4) after photoexcitation with a femtosecond pulse of 1.5 eV radiation. Complete melting of antiferromagnetic spin order is evidenced by the disappearance of a (1/4,1/4,1/2) diffraction peak. On the other hand, the (1/4,1/4,0) diffraction peak, reflecting orbital order, is only partially reduced. We interpret the results as evidence of destabilization in the short-range exchange pattern with no significant relaxation of the long-range Jahn-Teller distortions. Cluster calculations are used to analyze different possible magnetically ordered states in the long-lived metastable phase. Nonthermal coupling between light and magnetism emerges as a primary aspect of photoinduced phase transitions in manganites.