No Arabic abstract
Spin-dependent electric dipole operators are investigated group-theoretically for the emergence of an electric dipole induced by a single spin or by two spins, where the spin dependences are completely classified up to the quadratic order. For a single spin, a product of spin operators behaves as an even-parity electric quadrupole operator, which differs from an odd-parity electric dipole. The lack of the inversion symmetry allows the even- and odd-parity mixing, which leads to the electric dipole described by the electric quadruple operators. Point-group tables are given for classification of the possible spin-dependent electric dipoles and for the qualitative analysis of multiferroic properties, such as an emergent electric dipole moment coexisting with a magnetic moment, electromagnon excitation, and directional dichroism. The results can be applied to a magnetic ion in crystals or embedded in molecules at a site without the inversion symmetry. In the presence of an inversion symmetry, the electric dipole does not appear for a single spin. This is not the case for the electric dipole induced by two spins with antisymmetric spin dependence, which is known as vector spin chirality, in the presence of the inversion center between the two spins. In the absence of the inversion center, symmetric spin-dependent electric dipoles are also relevant. The detailed analysis of various symmetries of two-spin states is applied to spin dimer systems and the related multiferroic properties.
Magnetoelectric effects in honeycomb antiferromagnet Co4Nb2O9 are investigated on the basis of symmetry analyses of Co ions in trigonal P-3c1 space group. For each Co ion, the possible spin dependence is classified by C3 point-group symmetry. This accounts for the observed main effect that an electric polarization rotates in the opposite direction at the twice speed relative to the rotation of the external magnetic field applied in the ab-plane. Inversion centers and twofold axes in the unit cell restrict the active spin-dependence of the electric polarization, which well explains the observed experimental results. Expected optical properties of quadrupolar excitation and various types of dichroism are also discussed.
The Haldane spin-chain compound, Tb2BaNiO5, with two antiferromagnetic transitions, one at T1=63K, and the other at T2=25K, has been recently shown by us to be an exotic multiferroic below T2. Here, we report the results of our investigations of Sr doping at the Ba site by magnetization, heat-capacity, magnetoelectric (MDE), and pyrocurrent measurements. An intriguing finding, which we stress, is that the ferroelectricity is lost even for a doping level of 10 atomic percent, though magnetic ordering prevails. The doped specimens however retain significant magnetodielectric behaviour, but with reduced magnitudes and qualitative changes with respect to the behaviour of the parent compound. This implies that ferroelectric order is also crucial for the anomalously large MDE in the parent compound, in addition to the role of 4f single-ion anisotropy.
An indispensable step to understand collective magnetic phenomena in rare-earth compounds is the determination of spatially-anisotropic single-ion properties resulting from spin-orbit coupling and crystal field (CF). The CF Hamiltonian has a discrete energy spectrum -- accessible to spectroscopic probes such as neutron scattering -- controlled by a number of independent parameters reflecting the point-symmetry of the magnetic sites. Determining these parameters in low-symmetry systems is often challenging. Here, we describe a general method to analyze CF excitation spectra using adjustable effective point-charges. We benchmark our method to existing neutron-scattering measurements on pyrochlore rare-earth oxides and obtain a universal point-charge model that describes a large family of related materials. We adapt this model to the newly discovered tripod Kagome magnets ($R_{3}$Mg$_2$Sb$_{3}$O$_{14}$, $R$ = Tb, Ho, Er, Yb) for which we report broadband inelastic neutron-scattering spectra. Analysis of these data using adjustable point-charges yields the CF wave-functions for each compound. From this, we calculate thermomagnetic properties that accurately reflect our measurements on powder samples, and predict the effective gyromagnetic tensor for pseudo-spin degrees of freedom -- a crucial step to understand the exotic collective properties of these kagome magnets at low temperature. We present further applications of our method to other tripod kagome materials and triangular rare-earth compounds $R$MgGaO$_4$ ($R$ =Yb, Tm). Overall, this study establishes a widely applicable methodology to predict CF and single-ion properties of rare-earth compounds based on interpretable and adjustable models of effective point-charges.
We incorporate single crystal Fe$_3$O$_4$ thin films into a gated device structure and demonstrate the ability to control the Verwey transition with static electric fields. The Verwey transition temperature ($T_V$) increases for both polarities of the electric field, indicating the effect is not driven by changes in carrier concentration. Energetics of induced electric polarization and/or strain within the Fe$_3$O$_4$ film provide a possible explanation for this behavior. Electric field control of the Verwey transition leads directly to a large magnetoelectric effect with coefficient of 585 pT m/V.
The honeycomb antiferromagnet Co4Nb2O9 is known to exhibit an interesting magnetoelectric effect that the electric polarization rotates at the twice speed in the opposite direction relative to the rotation of the external magnetic field applied in the basal ab-plane. The spin-dependent electric dipole can be an origin of the magnetoelectric effect. It is described by the product of spin operators at different sites (type-I theory) or at the same site (type-II theory). We examine the electric polarization for the two cases on the basis of the symmetry analysis of the crystal structure of Co4Nb2O9, and conclude that the latter is the origin of the observed result. This paper also gives a general description of the field-induced electric polarization on honeycomb lattices with the C3 point group symmetry on the basis of the type-I theory.