Multiferroics where at least two primary ferroic orders are present and coupled in a single system constitute an important class of materials. They attracted special consideration as they present both intriguing fundamental physics problems and technological importance for potential multifunctional devices. Here, we present the evidence of multiferroicity and magnetoelectric (ME) coupling in -Mn2O3; a unique binary perovskite. Corresponding to the antiferromagnetic (AFM) ordering around 80K, a clear frequency independent transition is observed in the dielectric permittivity. We showed that electric polarization emerges near AFM regime that can be modulated with magnetic field. The detailed structural analysis using synchrotron radiation X-ray diffraction demonstrates the increase in structural distortion with decreasing temperature, as well as changes in the unit cell parameters and bond lengths across the ferroelectric and magnetic ordering temperatures. This observation of multiferroicity and magnetoelastic coupling in -Mn2O3 provides insights for the exploration of ME coupling in related materials.

Simultaneous co-existence of room-temperature(T) ferromagnetism and ferroelectricity in Fe doped BaTiO3 (BTO) is intriguing, as such Fe doping into tetragonal BTO, a room-T ferroelectric (FE), results in the stabilization of its hexagonal polymorph which is FE only below ∼80K. Here, we investigate its origin and show that Fe-doped BTO has a mixed-phase room-temperature multiferroicity, where the ferromagnetism comes from the majority hexagonal phase and a minority tetragonal phase gives rise to the observed weak ferroelectricity. In order to achieve majority tetragonal phase (responsible for room-T ferroelectricity) in Fe-doped BTO, we investigate the role of different parameters which primarily control the PE hexagonal phase stability over the FE tetragonal one and identify three major factors namely, the effect of ionic size, Jahn-Teller (J-T) distortions and oxygen vacancies (OVs), to be primarily responsible. The effect of ionic size which can be qualitatively represented using the Goldschmidt's tolerance (GT) factor seems to be the major dictating factor for the hexagonal phase stability. The understanding of these factors not only enables us to control them but also, achieve suitable co-doped BTO compound with enhanced room-T multiferroic properties.

The effect of Cr doping with nominal compositions Mn 2-x Cr x O 3 (0  x  0.10) has been undertaken to investigate its effect on structural, magnetic, dielectric and magnetoelectric properties. The Cr doping transformed the room temperature crystal structure from orthorhombic to cubic symmetry. Similar to -Mn 2 O 3 , two magnetic transitions have been observed in the Cr doped samples. The effect of Cr doping is significant on the low temperature transition i.e. the lower magnetic transition shifted towards higher temperature (25 K for pristine to 40 K for x=0.10) whereas the high temperature transition decreases slightly with increasing Cr content. A clear frequency independent transition is observed in complex dielectric measurements for all compositions around high temperature magnetic ordering. Interestingly, the magnetodielectric behaviour enhanced enormously 21% with Cr substitution as compared to pristine Mn 2 O 3 .

We report the modifications in the electronic properties of single phase polycrystalline BaTiO3 due to ferroelectric to paraelectric phase transition revealed by temperature dependent synchrotron based x-ray absorption and valence band spectroscopy. Valence band spectra show a strong temperature dependence of Ti-3d and O-2p hybridized states around the phase transition. It is observed that Ti-O hybridization is stronger in the paraelectric phase, which is also supported by multiplet calculations at the Ti L-edge. We also find a reduced crystal field value in the paraelectric phase than in the ferroelectric phase, which is caused by volume expansion and a reduction in tetragonal distortion.

The effect of Sr doping in BaTiO 3 (BTO) with nominal compositions Ba 0.80 Sr 0.20 TiO 3 (BSTO) have been explored in its structural, lattice vibration, dielectric, ferroelectric and electrocaloric properties. The temperature dependent dielectric results elucidate the enhancement in dielectric constant and exhibit three frequency independent transitions around 335, 250 and 185 K which are related to different structural transitions. All these transitions occur at lower temperature as compared with pristine BTO, however; remnant electric polarization (P) of BSTO is much higher than in BTO. The value of P is  5C/cm 2 at room temperature and the maximum P 8C/cm 2 is observed at tetragonal to orthorhombic and orthorhombic to rhombohedral transitions. The electro-caloric effect shows the maximum adiabatic change in temperature T 0.24 K at cubic to tetragonal transition. The temperature dependent synchrotron X-ray diffraction and Raman results shows correlations between P, crystal structure and lattice vibrations. Our results demonstrate the enhancement in ferroelectric properties of BTO with Sr doping. The origin of the enhancement in ferroelectric property is also discussed which is related to the appearance of superlattice peak around room temperature due to TiO 6 octahedral distortion. These enhanced properties would be useful to design lead free high quality ferroelectric and piezoelectric materials.

Fe doping into BaTiO3 stabilizes the paraelectric hexagonal phase in place of the ferroelectric tetragonal one. We show that simultaneous doping of Bi along with Fe into BaTiO3 effectively enhances the magnetoelectric (ME) multiferroic response (both ferromagnetism and ferroelectricity) at room temperature, through careful tuning of Fe valency along with the controlled recovery of the ferroelectric-tetragonal phase. We also report a systematic increase in large dielectric constant values as well as reduction in loss tangent values with relatively moderate temperature variation of the dielectric constant around room temperature with increasing Bi doping content in Ba1−xBixTi0.90Fe0.10O3 (0 ≤ x ≤ 0.10), which makes the higher Bi–Fe codoped sample (x = 0.08) promising for use as a room-temperature high-κ dielectric material. Interestingly, the x = 0.08 (Bi–Fe codoped) sample is not only found to be ferroelectrically (∼20 times) and ferromagnetically (∼6 times) stronger than x = 0 (only Fe-doped) at room temperature, but also observed to be better insulating (larger bandgap) with indirect signatures of larger ME coupling as indicated from anomalous reduction of the magnetic coercive field with decreasing temperature. Thus, room-temperature ME multiferroicity has been engineered in Bi and Fe codoped BTO (BaTiO3) compounds.

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