No Arabic abstract
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.
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.
I show that a nonequilibrium paraelectric to ferroelectric transition can be induced using midinfrared pulses. This relies on a quartic $lQ_{textrm{l$_z$}}^2Q_{textrm{h$_x$}}^2$ coupling between the lowest ($Q_{textrm{l$_z$}}$) and highest ($Q_{textrm{h$_x$}}$) frequency infrared-active phonon modes of a paraelectric material. Density functional calculations show that the coupling constant $l$ is negative, which causes a softening of the $Q_{textrm{l$_z$}}$ mode when the $Q_{textrm{h$_x$}}$ mode is externally pumped. A rectification along the $Q_{textrm{l$_z$}}$ coordinate that stabilizes the nonequilibrium ferroelectric state occurs only above a critical threshold for the electric field of the pump pulse, demonstrating that this is a nonperturbative phenomenon. A first principles calculation of the coupling between light and the $Q_{textrm{h$_x$}}$ mode shows that ferroelectricity can be induced in the representative case of strained KTaO$_3$ by a midinfrared pulse with a peak electric field of 17 MV cm$^{-1}$ and duration of 2 ps. Furthermore, other odd-order nonlinear couplings make it possible to arbitrarily switch off the light-induced ferroelectric state, making this technique feasible for all-optic devices.
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.
Cubic spinel GeNi2O4 exhibits intriguing magnetic properties with two successive antiferromagnetic phase transitions (TN1 12.1 and TN2 11.4 K) with the absence of any structural transition. We have performed detailed heat capacity and magnetic measurements in different crystallographic orientations. A new magnetic phase in presence of magnetic field (H > 4 T) along the [111] direction is revealed, which is not observed when the magnetic field is applied along the [100] and [110] directions. High field neutron powder diffraction measurements confirm such a change in magnetic phase, which could be ascribed to a spin reorientation in the presence of magnetic field. A strong magnetic anisotropy and competing magnetic interactions play a crucial role on the complex magnetic behavior in this cubic system.
We present magnetization and magnetostriction studies of the insulating perovskite LaCoO3 in magnetic fields approaching 100 T. In marked contrast with expectations from single-ion models, the data reveal two distinct first-order spin transitions and well-defined magnetization plateaux. The magnetization at the higher plateau is only about half the saturation value expected for spin-1 Co3+ ions. These findings strongly suggest collective behavior induced by strong interactions between different electronic -- and therefore spin -- configurations of Co3+ ions. We propose a model of these interactions that predicts crystalline spin textures and a cascade of four magnetic phase transitions at high fields, of which the first two account for the experimental data.