By performing density functional calculations, we investigate the origin of the Skyrmion state and ferroelectricity in Cu2OSeO3. We find that the Dzyaloshinskii-Moriya interactions between the two different kinds of Cu ions are extremely strong and induce the helical ground state and the Skyrmion state in the absence and presence of a magnetic field, respectively. On the basis of the general model for the spin-order induced polarization, we propose that the ferroelectric polarization of Cu2OSeO3 in the collinear ferrimagnetic state arises from an unusual mechanism, i.e., the single-spin-site contribution due to the spin-orbit coupling.

A first-principles approach called the self-consistent quasiharmonic approximation (SC-QHA) method is formulated to calculate the thermal expansion, thermomechanics, and thermodynamic functions of solids at finite temperatures with both high efficiency and accuracy. The SC-QHA method requires fewer phonon calculations than the conventional QHA method, and also facilitates the convenient analysis of the microscopic origins of macroscopic thermal phenomena. The superior performance of the SC-QHA method is systematically examined by comparing it with the conventional QHA method and experimental measurements on silicon, diamond, and alumina. It is then used to study the effects of pressure on the anharmonic lattice properties of diamond and alumina. The thermal expansion and thermomechanics of Ca3Ti2O7, which is a recently discovered important ferroelectric ceramic with a complex crystal structure that is computationally challenging for the conventional QHA method, are also calculated using the formulated SC-QHA method. The SC-QHA method can significantly reduce the computational expense for various quasiharmonic thermal properties especially when there are a large number of structures to consider or when the solid is structurally complex. It is anticipated that the algorithm will be useful for a variety of fields, including oxidation, corrosion, high-pressure physics, ferroelectrics, and high-throughput structure screening when temperature effects are required to accurately describe realistic properties.

By extending our general spin-current model to non-centrosymmetric spin dimers and performing density functional calculations, we investigate the causes for the helical magnetic order and the origin of the giant ferroelectric polarization of CaMn 7 O 12 . The giant ferroelectric polarization is proposed to be caused by the symmetric exchange striction due to the canting of the Mn 4+ spin arising from its strong Dzyaloshinskii-Moriya (DM) interaction. Our study suggests that CaMn 7 O 12 may exhibit a novel magnetoelectric coupling mechanism in which the magnitude of the polarization is governed by the exchange striction, but the direction of the polarization by the chirality of the helical magnetic order.

We use polarized neutron scattering to demonstrate that in-plane spin excitations in electron doped superconducting BaFe1.904Ni0.096As2 (Tc=19.8  K) change from isotropic to anisotropic in the tetragonal phase well above the antiferromagnetic (AFM) ordering and tetragonal-to-orthorhombic lattice distortion temperatures (TN≈Ts=33±2  K) without an uniaxial pressure. While the anisotropic spin excitations are not sensitive to the AFM order and tetragonal-to-orthorhombic lattice distortion, superconductivity induces further anisotropy for spin excitations along the [110] and [110] directions. These results indicate that the spin excitation anisotropy is a probe of the electronic anisotropy or orbital ordering in the tetragonal phase of iron pnictides.