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Debraj Choudhury

Publications and source records attributed to Debraj Choudhury.

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Antisite-disorder driven tuning of magnetic properties and exchange-bias in Nd$_{2-x}$Sr$_{x}$CoMnO$_{6-\delta}$ $(0 \leq x \leq 1)$ ($\delta \sim 0.5$) double perovskites

We demonstrate precise control of exchange bias (EB) in the Nd$_{2-x}$Sr$_x$CoMnO$_{6-\delta}$ ($0 \leq x \leq 1$) double-perovskite series through Sr$^{2+}$ induced hole doping, unveiling a remarkable transition between normal and inverse EB states. Employing neutron powder diffraction and X-ray absorption spectroscopy, we reveal a structural evolution from a B-site-ordered monoclinic ($P2_1/n$) phase to a disordered rhombohedral ($R\overline{3}c$) phase with increasing $x$, accompanied by a shift in the effective Co valence from +2 toward +3, while the Mn valence remains essentially unchanged. DC magnetization measurements indicate a gradual suppression of ferromagnetism with hole doping, whereas AC susceptibility measurements at $x = 0.75$ reveal pronounced cluster-glass behavior and the highest EB field of $\sim 4$ kOe at 8 K under a 6 T cooling field. After correcting for minor-loop effects, we identify robust inverse EB at $x = 0.75$, persisting even under a cooling field of 6 T. We attribute this phenomenon to competing ferromagnetic--antiferromagnetic and ferromagnetic--glassy interfaces, governed by strong magnetic frustration and the magnetocrystalline anisotropy associated with rare-earth 4$f$ electrons. These findings elucidate the pivotal role of doping-induced structural and magnetic competition in tailoring EB behavior in rare-earth double perovskites, providing new insights for the design of advanced magnetic materials.

cond-mat.str-el

Emergent room-temperature ferroelectricity in spark-plasma sintered DyCrO$_3$ and LaCrO$_3$

Identification of novel multiferroic materials with high-ordering temperatures remains at the forefront of condensed matter physics research. In this regard, the antiferromagnetic RCrO$_3$ compounds (like GdCrO$_3$) constitute a promising class of multiferroic compounds, which, however, mostly become ferroelectric concomitant with the antiferromagnetic ordering much below room-temperature, arising from a subtle competition between the ferroelectric off-centering mode and a non-polar antiferrodistortive rotation mode that inhibits ferroelectricity. Recently, room-temperature ferroelectricity of structural origin, arising from off-centering displacements of R and Cr ions, has been identified in spark-plasma sintered GdCrO$_3$ [Suryakanta Mishra et al., Phys. Rev. B 104, L180101 (2021)]. Interestingly, some of the experimentally observed non-ferroelectric RCrO$_3$ compounds have been theoretically predicted to host similar ferroelectric instabilities. Here, we have identified two such non-ferroelectric RCrO3 compounds, one DyCrO$_3$ (which is reported as a quantum paraelectric) and another LaCrO$_3$ (which is paraelectric), and using a modified synthesis protocol involving spark-plasma-sintering (SPS), we have been successful in engineering an intrinsic room-temperature ferroelectricity in the paramagnetic state, driven by noncentrosymmetric structural phase in both SPS sintered DyCrO$_3$ and LaCrO$_3$, in contrast to room-temperature paraelectricity in solid-state synthesized DyCrO$_3$ and LaCrO$_3$. While the ferroelectricity in SPS-prepared DyCrO$_3$ and LaCrO$_3$ is stable at room-temperature, it undergoes an irreversible transition from a ferroelectric (Pna2$_1$) phase to a paraelectric (Pbnm) phase at 440 K. Significantly, SPS-sintered LaCrO$_3$, which undergoes antiferromagnetic ordering at 290 K, emerges as a promising near room-temperature multiferroic material.

cond-mat.mtrl-sci

Engineering room-temperature multiferroicity in Bi and Fe codoped BaTiO3

Fe doping into BaTiO3, stabilizes the paraelectric hexagonal phase in place of the ferroelectric tetragonal one [P. Pal et al. Phys. Rev. B, 101, 064409 (2020)]. 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 ferroelectric-tetragonal phase. We also report systematic increase in large dielectric constant values as well as reduction in loss tangent values with relatively moderate temperature variation of dielectric constant around room-temperature with increasing Bi doping content in Ba1-xBixTi0.9Fe0.1O3 (0<x<0.1), which makes the higher Bi-Fe codoped sample (x=0.08) promising for the use as room-temperature high-k dielectric material. Interestingly, 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 magnetic coercive field with decreasing temperature. Thus, room-temperature ME multiferroicity has been engineered in Bi and Fe codoped BTO (BaTiO3) compounds.

cond-mat.mtrl-sci

Origin and tuning of room-temperature multiferroicity in Fe doped BaTiO$_3$

Simultaneous co-existence of room-temperature(T) ferromagnetism and ferroelectricity in Fe doped BaTiO$_3$ (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 $\sim$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.

cond-mat.mtrl-sci

Electric and magnetic polarizabilities of hexagonal Ln2CuTiO6 (Ln=Y, Dy, Ho, Er and Yb)

We investigated the rare-earth transition metal oxide series, Ln2CuTiO6 (Ln=Y, Dy, Ho, Er and Yb), crystallizing in the hexagonal structure with non-centrosymmetric P63cm space group for possible occurrences of multiferroic properties. Our results show that while these compounds, except Ln=Y, exhibit a low temperature antiferromagnetic transition due to the ordering of the rare-earth moments, the expected ferroelectric transition is frustrated by the large size difference between Cu and Ti at the B-site. Interestingly, this leads these compounds to attain a rare and unique combination of desirable paraelectric properties with high dielectric constants, low losses and weak temperature and frequency dependencies. First-principles calculations establish these exceptional properties result from a combination of two effects. A significant difference in the MO5 polyhedral sizes for M = Cu and M = Ti suppress the expected co-operative tilt pattern of these polyhedra, required for the ferroelectric transition, leading to relatively large values of the dielectric constant for every compound investigated in this series. Additionally, it is shown that the majority contribution to the dielectric constant arises from intermediate-frequency polar vibrational modes, making it relatively stable against any temperature variation. Changes in the temperature stability of the dielectric constant amongst different members of this series are shown to arise from changes in relative contributions from soft polar modes.

cond-mat.mtrl-sci