Tuning magnetoelectricity in a mixed-anisotropy antiferromagnet.

Control of magnetization and electric polarization is attractive in relation to tailoring materials for data storage and devices such as sensors or antennae. In magnetoelectric materials, these degrees of freedom are closely coupled, allowing polarization to be controlled by a magnetic field, and magnetization by an electric field, but the magnitude of the effect remains a challenge in the case of single-phase magnetoelectrics for applications. We demonstrate that the magnetoelectric properties of the mixed-anisotropy antiferromagnet LiNi1-xFexPO4 are profoundly affected by partial substitution of Ni2+ ions with Fe2+ on the transition metal site. This introduces random site-dependent single-ion anisotropy energies and causes a lowering of the magnetic symmetry of the system. In turn, magnetoelectric couplings that are symmetry-forbidden in the parent compounds, LiNiPO4 and LiFePO4, are unlocked and the dominant coupling is enhanced by almost two orders of magnitude. Our results demonstrate the potential of mixed-anisotropy magnets for tuning magnetoelectric properties.

Preferred Spin Excitations in the Bilayer Iron-Based Superconductor CaK(Fe_{0.96}Ni_{0.04})_{4}As_{4} with Spin-Vortex Crystal Order.

Spin-orbit coupling (SOC) is a key to understand the magnetically driven superconductivity in iron-based superconductors, where both local and itinerant electrons are present and the orbital angular momentum is not completely quenched. Here, we report a neutron scattering study on the bilayer compound CaK(Fe_{0.96}Ni_{0.04})_{4}As_{4} with superconductivity coexisting with a noncollinear spin-vortex crystal magnetic order that preserves the tetragonal symmetry of the Fe-Fe plane. In the superconducting state, two spin resonance modes with odd and even L symmetries due to the bilayer coupling are found similar to the undoped compound CaKFe_{4}As_{4} but at lower energies. Polarization analysis reveals that the odd mode is c-axis polarized, and the low-energy spin anisotropy can persist to the paramagnetic phase at high temperature, which closely resembles other systems with in-plane collinear and c-axis biaxial magnetic orders. These results provide the missing piece of the puzzle on the SOC effect in iron-pnictide superconductors, and also establish a common picture of c-axis preferred magnetic excitations below T_{c} regardless of the details of magnetic pattern or lattice symmetry.

Field-Induced Modulated State in the Ferromagnet PrPtAl.

The theory of quantum order-by-disorder (QOBD) explains the formation of modulated magnetic states at the boundary between ferromagnetism and paramagnetism in zero field. PrPtAl has been argued to provide an archetype for this. Here, we report the phase diagram in magnetic field, applied along both the easy a axis and hard b axis. For field aligned to the b axis, we find that the magnetic transition temperatures are suppressed and at low temperature there is a single modulated fan state, separating an easy a axis ferromagnetic state from a field polarized state. This fan state is well explained with the QOBD theory in the presence of anisotropy and field. Experimental evidence supporting the QOBD explanation is provided by the large increase in the T^{2} coefficient of the resistivity and direct detection of enhanced magnetic fluctuations with inelastic neutron scattering, across the field range spanned by the fan state. This shows that the QOBD mechanism can explain field induced modulated states that persist to very low temperature.

Magnetization Density Distribution of Sr_{2}IrO_{4}: Deviation from a Local j_{eff}=1/2 Picture.

5d iridium oxides are of huge interest due to the potential for new quantum states driven by strong spin-orbit coupling. The strontium iridate Sr_{2}IrO_{4} is particularly in the spotlight because of the so-called j_{eff}=1/2 state consisting of a quantum superposition of the three local t_{2g} orbitals with, in its simplest version, nearly equal populations, which stabilizes an unconventional Mott insulating state. Here, we report an anisotropic and aspherical magnetization density distribution measured by polarized neutron diffraction in a magnetic field up to 5 T at 4 K, which strongly deviates from a local j_{eff}=1/2 picture even when distortion-induced deviations from the equal weights of the orbital populations are taken into account. Once reconstructed by the maximum entropy method and multipole expansion model refinement, the magnetization density shows four cross-shaped positive lobes along the crystallographic tetragonal axes with a large spatial extent, showing that the xy orbital contribution is dominant. The analogy to the superconducting copper oxide systems might then be weaker than commonly thought.

Coexistence of Ferromagnetic and Stripe Antiferromagnetic Spin Fluctuations in SrCo_{2}As_{2}.

We use inelastic neutron scattering to study energy and wave vector dependence of spin fluctuations in SrCo_{2}As_{2}, derived from SrFe_{2-x}Co_{x}As_{2} iron pnictide superconductors. Our data reveal the coexistence of antiferromagnetic (AF) and ferromagnetic (FM) spin fluctuations at wave vectors Q_{AF}=(1,0) and Q_{FM}=(0,0)/(2,0), respectively. By comparing neutron scattering results with those of dynamic mean field theory calculation and angle-resolved photoemission spectroscopy experiments, we conclude that both AF and FM spin fluctuations in SrCo_{2}As_{2} are closely associated with a flatband of the e_{g} orbitals near the Fermi level, different from the t_{2g} orbitals in superconducting SrFe_{2-x}Co_{x}As_{2}. Therefore, Co substitution in SrFe_{2-x}Co_{x}As_{2} induces a t_{2g} to e_{g} orbital switching, and is responsible for FM spin fluctuations detrimental to the singlet pairing superconductivity.

Low-energy spin dynamics of orthoferrites AFeO3 (A = Y, La, Bi).

YFeO3 and LaFeO3 are members of the rare-earth orthoferrites family with Pbnm space group. Using inelastic neutron scattering, the low-energy spin excitations have been measured around the magnetic Brillouin zone center. Splitting of magnon branches and finite magnon gaps (∼2 meV) are observed for both compounds, where the Dzyaloshinsky-Moriya interactions account for most of this gap with some additional contribution from single-ion anisotropy. We also make comparisons with multiferroic BiFeO3 (R3c space group), in which similar behavior was observed. By taking into account all relevant local Dzyaloshinsky-Moriya interactions, our analysis allows for the precise determination of all experimentally observed parameters in the spin-Hamiltonian. We find that different properties of the Pbnm and R3c space group lead to the stabilization of a spin cycloid structure in the latter case but not in the former, which explains the difference in the levels of complexity of magnon band structures for the respective compounds.

Time-reversal symmetry breaking hidden order in Sr2(Ir,Rh)O4.

Layered 5d transition iridium oxides, Sr2(Ir,Rh)O4, are described as unconventional Mott insulators with strong spin-orbit coupling. The undoped compound, Sr2IrO4, is a nearly ideal two-dimensional pseudospin-1/2 Heisenberg antiferromagnet, similarly to the insulating parent compound of high-temperature superconducting copper oxides. Using polarized neutron diffraction, we here report a hidden magnetic order in pure and doped Sr2(Ir,Rh)O4, distinct from the usual antiferromagnetic pseudospin ordering. We find that time-reversal symmetry is broken while the lattice translation invariance is preserved in the hidden order phase. The onset temperature matches that of the odd-parity hidden order recently highlighted using optical second-harmonic generation experiments. The novel magnetic order and broken symmetries can be explained by the loop-current model, previously predicted for the copper oxide superconductors.

a-b Anisotropy of the Intra-Unit-Cell Magnetic Order in YBa_{2}Cu_{3}O_{6.6}.

Within the complex phase diagram of the hole-doped cuprates, seizing the nature of the mysterious pseudogap phase is essential for unraveling the microscopic origin of high-temperature superconductivity. Below the pseudogap temperature T^{⋆}, evidence for intra-unit-cell orders breaking the fourfold rotation symmetry have been provided by neutron diffraction and scanning tunneling spectroscopy. Using polarized neutron diffraction on a detwinned YBa_{2}Cu_{3}O_{6.6} sample, we here report a distinct a-b anisotropy of the intra-unit-cell magnetic structure factor below T^{⋆}, highlighting that intra-unit-cell order in this material breaks the mirror symmetry of the CuO_{2} bilayers. This is likely to originate from a crisscrossed arrangement of loop currents within the CuO_{2} bilayer, resulting in a bilayer mean toroidal axis along the b direction.

Elastic Constants, Optical Phonons, and Molecular Relaxations in the High Temperature Plastic Phase of the CH3NH3PbBr3 Hybrid Perovskite.

Low frequency dynamics has been studied in a CH3NH3PbBr3 hybrid perovskite single crystal by using four different spectroscopy techniques: coherent inelastic neutron, Raman and Brillouin scatterings, and ultrasound measurements. Sound velocities were measured over five decades in energy to yield the complete set of elastic constants in a hybrid halide perovskite crystal in the pseudocubic plastic phase. The C44 shear elastic constant is very small, leading to a particularly low resistance to shear stress. Brillouin scattering has been used to study the relaxation dynamics of methylammonium cations and to evidence translation-rotation coupling associated with the cubic to tetragonal phase transition at Tc ≈ 230 K. Low frequency and highly damped optical phonons observed using both Raman and inelastic neutron below 18 meV, do not present softening close to Tc. The critical dynamics at Tc ≈ 230 K is compatible with an order-disorder character, dominated by relaxational motions of the molecules.

Hidden degrees of freedom in aperiodic materials.

Numerous crystalline materials, including those of bioorganic origin, comprise incommensurate sublattices whose mutual arrangement is described in a superspace framework exceeding three dimensions. We report direct observation by neutron diffraction of superspace symmetry breaking in a solid-solid phase transition of an incommensurate host-guest system: the channel inclusion compound of nonadecane/urea. Strikingly, this phase transition generates a unit cell doubling that concerns only the modulation of one substructure by the other-an internal variable available only in superspace. This unanticipated pathway for degrees of freedom to rearrange leads to a second phase transition, which again is controlled by the higher dimensionality of superspace. These results reveal nature's capacity to explore the increased number of phases allowed in aperiodic crystals.

Interactions in self-organized nanoporous organic crystals.

This Letter reports on the structural analysis of a self-assembly material, the prototype host-guest urea-alkane nanoporous crystal. Different spectroscopic techniques, under hydrostatic pressure, reveal a totally unexpected ordered phase where ordering does not require any apparent deformation of the host. This fundamental observation raises the question of the actual interactions in other similar supramolecular or biological tubular systems.

First one-dimensional stress-strain experiments inside an aperiodic inclusion compound: evidence of depinning effects.

This Letter reports on the first observation of depinning under hydrostatic pressure of the guest and host sublattices inside the aperiodic nonadecane-urea inclusion compound. This leads to a unique way for a direct determination of the one-dimensional interguest interaction (1 N/m for nonadecane).