No Arabic abstract
We demonstrate that small but finite ferroelectric polarization ($sim$0.01 $mu$C/cm$^2$) emerges in orthorhombic LuFeO$_3$ ($Pnma$) at $T_N$ ($sim$600 K) because of commensurate (k = 0) and collinear magnetic structure. The synchrotron x-ray and neutron diffraction data suggest that the polarization could originate from enhanced bond covalency together with subtle contribution from lattice. The theoretical calculations indicate enhancement of bond covalency as well as the possibility of structural transition to the polar $Pna2_1$ phase below $T_N$. The $Pna2_1$ phase, in fact, is found to be energetically favorable below $T_N$ in orthorhombic LuFeO$_3$ ($albeit$ with very small energy difference) than in isostructural and nonferroelectric LaFeO$_3$ or NdFeO$_3$. Application of electric field induces finite piezostriction in LuFeO$_3$ via electrostriction resulting in clear domain contrast images in piezoresponse force microscopy.
The origin of electromagnon excitations in cycloidal textit{R}MnO$_3$ is explained in terms of the Heisenberg coupling between spins despite the fact that the static polarization arises from the much weaker Dzyaloshinskii-Moriya (DM) exchange interaction. We present a model that incorporates structural characteristics of this family of manganites that is confirmed by far infrared transmission data as a function of temperature and magnetic field and inelastic neutron scattering results. A deep connection is found between the magnetoelectric dynamics of the spiral phase and the static magnetoelectric coupling in the collinear E-phase of this family of manganites.
The magnetic structures which endow TbMnO$_3$ with its multiferroic properties have been reassessed on the basis of a comprehensive soft x-ray resonant scattering (XRS) study. The selectivity of XRS facilitated separation of the various contributions (Mn $L_2$ edge, Mn 3d moments; Tb M$_4$ edge, Tb 4f moments), while its variation with azimuth provided information on the moment direction of distinct Fourier components. When the data are combined with a detailed group theory analysis, a new picture emerges of the ferroelectric transition at 28 K. Instead of being driven by the transition from a collinear to a non-collinear magnetic structure, as has previously been supposed, it is shown to occur between two non-collinear structures.
We have performed ab initio calculations within the LDA+U method in the multilayered system (LaMnO$_3$)$_{2n}$ / (SrMnO$_3$)$_n$. Our results suggest a charge-ordered state that alternates Mn$^{3+}$ and Mn$^{4+}$ cations in a checkerboard in-plane pattern is developed at the interfacial layer, leading to a gap opening. Such an interfacial charge-ordered situation would be the energetically favored reconstruction between LaMnO$_3$ and SrMnO$_3$. This helps understanding the insulating behavior observed experimentally in these multilayers at intermediate values of $n$, whose origin is known to be due to some interfacial mechanism.
This work shows an unconventional route for spin-driven ferroelectricity originating from a metastable magnetic field-induced canting of chromium sublattice in the presence of gadolinium moments in GdCrTiO5 at low temperatures. Compared to the isostructural neodymium compound, significant differences of magnetism and magnetoelectric effects are seen. We present the results of thorough investigations of temperature and magnetic field dependent magnetization as well as ac and dc magnetic susceptibility. These bulk measurements are complemented by local-probe spectroscopy utilizing electron-spin resonance and muon-spin rotation/relaxation for probing the chromium moments. Ferroelectric order is inferred from pyro- and magnetocurrent measurements. GdCrTiO5 shows a pyrocurrent signal around 10 K, only if the system is cooled in an applied magnetic field exceeding 10 kOe. A distinct spin-driven ferroelectric order is revealed in this state for temperatures below 10 K, which can be switched by changing magnetic-field direction and the polarity of the electric field. But, the magnetic measurements reveal no clear signature of long-range magnetic ordering. The presence of such meta-magnetoelectric-type behaviour in the absence of any meta-magnetic behavior is rare in the literature. Our microscopic spectroscopy results indicate significant changes of the magnetic properties around 10 K. Probably there is an exchange frustration between Gd and Cr moments, which prevents long-range magnetic ordering at further high temperature. Below 10 K, weak magnetic ordering occurs by minimizing frustration due to lattice distortion, which helps in magnetodielectric coupling. However, the non-polar distortion attains appreciable values after application of magnetic fields above 10 kOe to break the spatial inversion symmetry, which creates ferroelectricity.
TbMnO3 is an orthorhombic insulator where incommensurate spin order for temperature T_N < 41K is accompanied by ferroelectric order for T < 28K. To understand this, we establish the magnetic structure above and below the ferroelectric transition using neutron diffraction. In the paraelectric phase, the spin structure is incommensurate and longitudinally-modulated. In the ferroelectric phase, however, there is a transverse incommensurate spiral. We show that the spiral breaks spatial inversion symmetry and can account for magnetoelectricity in TbMnO3.