Magnetic chirality as probed by neutron scattering

We review the concept of chirality, at first briefly in a general context then in the specific framework of the spin networks. We next discuss to what extent neutron scattering appears as an unconvertible tool to probe magnetic chirality in the static and dynamical regimes of the spins. The remarkable chiral ground state and excitations of the Fe-langasite compound finally serves to illustrate the use of neutron polarimetry in the experimental studies of the magnetic chirality.Comment: 32 page

Spin liquid correlations in Nd-langasite anisotropic Kagom\'e antiferromagnet

Dynamical magnetic correlations in the geometrically frustrated Nd$\_3$Ga$\_5$SiO$\_{14}$ compound were probed by inelastic neutron scattering on a single crystal. A scattering signal with a ring shape distribution in reciprocal space and unprecedented dispersive features was discovered. Comparison with calculated static magnetic scattering from models of correlated spins suggests that the observed phase is a spin liquid inherent to an antiferromagnetic kagom\'e-like lattice of anisotropic Nd moments.Comment: 4 page

Magnetic order in the frustrated Ising-like chain compound Sr3_3NiIrO6_6

We have studied the field and temperature dependence of the magnetization of single crystals of Sr3NiIrO6. These measurements evidence the presence of an easy axis of anisotropy and two anomalies in the magnetic susceptibility. Neutron powder diffraction realized on a polycrystalline sample reveals the emergence of magnetic reflections below 75 K with magnetic propagation vector k ~ (0, 0, 1), undetected in previous neutron studies [T.N. Nguyen and H.-C zur Loye, J. Solid State Chem., 117, 300 (1995)]. The nature of the magnetic ground state, and the presence of two anomalies common to this family of material, are discussed on the basis of the results obtained by neutron diffraction, magnetization measurements, and symmetry arguments

Chemical decoration in cubic approximant and quasicrystal in the Al-Cu-Fe system

International audienceThe local order in the Al--Cu--Fe quasicrystal and in two of its approximants has been investigated by extended X-ray absorption fine structure (EXAFS) studies at the Cu and Fe Kedges. The chemical occupation of the crystallographic sites in the 1/1 cubic α--Al55Si7Cu25.5Fe12.5 phase is revisited. From these results, a model for the chemical short--range order in the Al62.5Cu25.5Fe 12.5 quasicrystal is proposed

Phase diagram of multiferroic KCu3_3As2_2O7_7(OD)3_3

The layered compound KCu$_3$As$_2$O$_7$(OD)$_3$, comprising distorted kagome planes of $S=1/2$ Cu$^{2+}$ ions, is a recent addition to the family of type-II multiferroics. Previous zero field neutron diffraction work has found two helically ordered regimes in \kns, each showing a distinct coupling between the magnetic and ferroelectric order parameters. Here, we extend this work to magnetic fields up to $20$~T using neutron powder diffraction, capacitance, polarization, and high-field magnetization measurements, hence determining the $H-T$ phase diagram. We find metamagnetic transitions in both low temperatures phases around $\mu_0 H_c \sim 3.7$~T, which neutron powder diffraction reveals to correspond to a rotation of the helix plane away from the easy plane, as well as a small change in the propagation vector. Furthermore, we show that the sign of the ferroelectric polarization is reversible in a magnetic field, although no change is observed (or expected on the basis of the magnetic structure) due to the transition at $3.7$~T. We finally justify the temperature dependence of the polarization in both zero-field ordered phases by a symmetry analysis of the free energy expansion

Parity Broken Chiral Spin Dynamics in Ba3_3NbFe3_3Si2_2O14_{14}

The spin wave excitations emerging from the chiral helically modulated 120$^{\circ}$ magnetic order in a langasite Ba$_3$NbFe$_3$Si$_2$O$_{14}$ enantiopure crystal were investigated by unpolarized and polarized inelastic neutron scattering. A dynamical fingerprint of the chiral ground state is obtained, singularized by (i) spectral weight asymmetries answerable to the structural chirality and (ii) a full chirality of the spin correlations observed over the whole energy spectrum. The intrinsic chiral nature of the spin waves elementary excitations is shown in absence of macroscopic time reversal symmetry breaking

THz Magneto-electric atomic rotations in the chiral compound Ba3_3NbFe3_3Si2_2O14_{14}

We have determined the terahertz spectrum of the chiral langasite Ba$_3$NbFe$_3$Si$_2$O$_{14}$ by means of synchrotron-radiation measurements. Two excitations are revealed that are shown to have a different nature. The first one, purely magnetic, is observed at low temperature in the magnetically ordered phase and is assigned to a magnon. The second one persits far into the paramagnetic phase and exhibits both an electric and a magnetic activity at slightly different energies. This magnetoelectric excitation is interpreted in terms of atomic rotations and requires a helical electric polarization

Vibronic collapse of ordered quadrupolar ice in the pyrochore magnet Tb2+x_{2+x}Ti2−x_{2-x}O7+y_{7+y}

While the spin liquid state in the frustrated pyrochlore Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ has been studied both experimentally and theoretically for more than two decades, no definite description of this unconventional state has been achieved. Using synchrotron based THz spectroscopy in combination with quantum numerical simulations, we highlight a significant link between two previously unrelated features: the existence of a quadrupolar order following an ice rule and the presence of strong magneto-elastic coupling in the form of hybridized Tb$^{3+}$ crystal-field and phonon modes. The magnitude of this so-called vibronic process, which involves quadrupolar degrees of freedom, is significantly dependent on small off-stoichiometry $x$ and favors all-in all-out like correlations between quadrupoles. This mechanism competes with the long range ordered quadrupolar ice, and for slightly different stoichiometry, is able to destabilize it.Comment: Main text: 7 pages, 3 figures ; Supplemental Material: 6 pages, 2 figure

Helical bunching and symmetry lowering inducing multiferroicity in Fe langasites

International audienceThe chiral Fe-based langasites represent model systems of triangle-based frustrated magnets with a strong potential for multiferroicity. We report neutron scattering measurements for the multichiral Ba3MFe3Si2O14 (M = Nb, Ta) langasites revealing new important features of the magnetic order of these systems: the bunching of the helical modulation along the c-axis and the in-plane distortion of the 120° Fe-spin arrangement. We discuss these subtle features in terms of the microscopic spin Hamiltonian, and provide the link to the magnetically-induced electric polarization observed in these systems. Thus, our findings put the multiferroicity of this attractive family of materials on solid ground

Lattice dynamics and spin excitations in the metal-organic framework [CH3_3NH3_3][Co(HCOO)3_3]

In metal-organic-framework (MOF) perovskites, both magnetic and ferroelectric orderings can be readily realized by compounding spin and charge degrees of freedom. The hydrogen bonds that bridge the magnetic framework and organic molecules have long been thought of as a key in generating multiferroic properties. However, the underlying physical mechanisms remain unclear. Here, we combine neutron diffraction, quasielastic and inelastic neutron scattering, and THz spectroscopy techniques to thoroughly investigate the dynamical properties of the multiferroic MOF candidate [CH$_3$NH$_3$][Co(HCOO)$_3$] through its multiple phase transitions. The wide range of energy resolutions reachable by these techniques enables us to scrutinize the coupling between the molecules and the framework throughout the phase transitions and interrogate a possible magnetoelectric coupling. Our results also reveal a structural change around 220 K which may be associated with the activation of a nodding donkey mode of the methylammonium molecule due to the ordering of the CH$_3$ groups. Upon the occurrence of the modulated phase transition around 130 K, the methylammonium molecules undergo a freezing of its reorientational motions which is concomitant with a change of the lattice parameters and anomalies of collective lattice vibrations. No significant change has been however observed in the lattice dynamics around the magnetic ordering, which therefore indicates the absence of a substantial magneto-electric coupling in zero-field