arXiv subjects

Hena Das

Publications and source records attributed to Hena Das.

At least 19 recordsLinked to original sources

arXiv2025

Charge Order Driven Multiferroic Behaviour in Sr$_4$Fe$_6$O$_{12}$: An $\textit{Ab-initio}$ Study

In this letter, we report the structural, electronic and ferroelectric properties of the layered mixed-valent transition-metal compound, Sr$_{4}$Fe$_{6}$O$_{12}$ (SFO). We demonstrate how SFO undergoes a phase transition from a high-temperature (T) centrosymmetric tetragonal phase ($P4_{2}/mnm$) to a low-T polar orthorhombic phase ($Pmn2_{1}$). The transition is primarily driven by charge ordering at tetrahedral Fe-layer creating Fe$^{3+}$ and Fe$^{2+}$ cations between two edge sharing tetrahedra. This charge ordering induces electronic polarization, which is remarkably larger (3.5 times) in magnitude than ionic polarization and oppositely directed, giving a net polarization of 0.05 C/m$^2$ which is comparable to the state-of-the-art rare-earth nickelets and manganite perovskites. The direction of structural distortion, governed by the polar mode irrep $Γ_{5}^{-}$, depends sensitively on the type of magnetic ordering in the Fe-octahedral layer. Consequently, both the ionic and electronic polarization directions are influenced by magnetic ordering, suggesting the potential for multiferroic behavior with strong magneto-electric coupling in this material.

cond-mat.str-el↗

arXiv2022

Coupling between improper ferroelectricity and ferrimagnetism in hexagonal ferrites

Antisymmetric Dzyaloshinskii-Moriya (DM) interactions generating from the spin-orbit coupling induce various fascinating properties, like magnetoelectric (ME) effect, weak ferromagnetism and non-trivial topological spin textures like skyrmions, in real materials. Compared to their symmetric isotropic exchange counterpart, these interactions are generally of a weaker order of strength, creating modest twisting in the spin structure which results in weak ferromagntism or weak linear ME effect. Our proposed two-sublattice model, in contrast, predicts a hitherto unobserved, charge ordered non-collinear ferrimagnetic behavior with a considerably high magnetization $\textbf{M}$ coexisting with a ferroelectric (FE) order with an electric polarization $\textbf{P}$ and a strong cross coupling between them which is primarily driven by the inter-sublattice DM interactions. The key to realize these effects is the coupling between these microscopic interactions and the FE primary order parameter. We predict microscopic mechanisms to achieve electric field $\textbf{E}$ induced spin-reorientation transitions and 180$^{\circ}$ switching of the direction of $\textbf{M}$. This model was realized in the hexagonal phase of LuFeO$_3$ doped with electrons. This system shows $P \sim$ 15 $μ$C/cm$^2$, $M \sim$ 1.3 $μ_B$/Fe and magnetic transition near room temperature ($\sim$ 290 K). Our theoretical results are expected to stimulate further quest for energy-efficient routes to control magnetism for spintronics applications.

cond-mat.mtrl-sci↗

arXiv2021

High-mobility two-dimensional carriers from surface Fermi arcs in magnetic Weyl semimetal films

High-mobility two-dimensional carriers originating from surface Fermi arcs in magnetic Weyl semimetals are highly desired for accessing exotic quantum transport phenomena and for topological electronics applications. Here, we demonstrate high-mobility two-dimensional carriers that show quantum oscillations in magnetic Weyl semimetal SrRuO3 epitaxial films by systematic angle-dependent, high-magnetic field magnetotransport experiments. The exceptionally high-quality SrRuO3 films were grown by state-of-the-art oxide thin film growth technologies driven by machine learning algorithm. The quantum oscillations for the 10-nm SrRuO3 film show a high quantum mobility of 3500 cm2/Vs, a light cyclotron mass, and two-dimensional angular dependence, which can be attributed to the surface Fermi arcs. The linear thickness dependence of the phase shift of the quantum oscillations provides evidence for the non-trivial nature of the quantum oscillations mediated by the surface Fermi arcs. In addition, at low temperatures and under magnetic fields of up to 52 T, the quantum limit of SrRuO3 manifests the chiral anomaly of the Weyl nodes. Emergence of the hitherto hidden two-dimensional Weyl states in a ferromagnetic oxide pave the way to explore novel quantum transport phenomena for topological oxide electronics.

cond-mat.mtrl-sci↗

arXiv2021

Exploring the possible origin of spin reorientation transition in NdCrO$_3$

Spin reorientation transitions and other related magnetic phenomena, which owe their origin to the complex interplay between multiple magnetic sublattices, have long attracted scientific attention both from the perspective of fundamental curiosity and technological applications. In this study, combining first principles calculations together with finite temperature Monte Carlo simulations, we explore the possible origins of reorientation transition of Cr spins in NdCrO$_3$. We construct a NdCrO$_3$ specific magnetic model, consisting of symmetric superexchange interactions between magnetic ions, as well as their magnetic anisotropy. We show that the observed spin reorientation in NdCrO$_3$, arises out of a delicate balance between Nd$-$Cr magnetic exchange interactions, single ion anisotropy of Nd spins, and single ion anisotropy of Cr spins. Moreover, though our model does not take into consideration the effect of anti-symmetric and anisotropic-symmetric magnetic exchanges, the qualitative as well as quantitative agreement of the theoretically derived and the experimentally observed spin-reorientation transition in NdCrO$_3$, confirms the merit of our proposed microscopic model. Our results also propose a hitherto unobserved collective magnetic ordering in Nd sublattice, which is challenging to detect as it is an extreme low temperature phenomena, therefore calls for further investigations.

cond-mat.mtrl-sci↗

arXiv2020

Quantum transport evidence of Weyl fermions in an epitaxial ferromagnetic oxide

Magnetic Weyl fermions, which occur in magnets, have novel transport phenomena related to pairs of Weyl nodes, and they are, of both, scientific and technological interest, with the potential for use in high-performance electronics, spintronics and quantum computing. Although magnetic Weyl fermions have been predicted to exist in various oxides, evidence for their existence in oxide materials remains elusive. SrRuO3, a 4d ferromagnetic metal often used as an epitaxial conducting layer in oxide heterostructures, provides a promising opportunity to seek for the existence of magnetic Weyl fermions. Advanced oxide thin film preparation techniques, driven by machine learning technologies, may allow access to such topological matter. Here we show direct quantum transport evidence of magnetic Weyl fermions in an epitaxial ferromagnetic oxide SrRuO3: unsaturated linear positive magnetoresistance (MR), chiral-anomaly-induced negative MR, Pi Berry phase accumulated along cyclotron orbits, light cyclotron masses and high quantum mobility of about 10000 cm2/Vs. We employed machine-learning-assisted molecular beam epitaxy (MBE) to synthesize SrRuO3 films whose quality is sufficiently high to probe their intrinsic quantum transport properties. We also clarified the disorder dependence of the transport of the magnetic Weyl fermions, and provided a brand-new diagram for the Weyl transport, which gives a clear guideline for accessing the topologically nontrivial transport phenomena. Our results establish SrRuO3 as a magnetic Weyl semimetal and topological oxide electronics as a new research field.

cond-mat.mtrl-sci↗

arXiv2018

An L$_0$L$_1$-norm compressive sensing paradigm for the construction of sparse predictive lattice models using mixed integer quadratic programming

First-principles based lattice models allow the modeling of ab initio thermodynamics of crystalline mixtures for applications such as the construction of phase diagrams and the identification of ground state atomic orderings. The recent development of compressive sensing approaches for the construction of lattice models has further enabled the systematic construction of sparse physical models without the need for human intuition other than requiring the compactness of effective cluster interactions. However, conventional compressive sensing based on L1-norm regularization is strictly only applicable to certain classes of optimization problems and is otherwise not guaranteed to generate optimally sparse and transferable results, so that the method can only be applied to some materials science applications. In this paper, we illustrate a more robust L0L1-norm compressive-sensing method that removes the limitations of conventional compressive sensing and generally results in sparser lattice models that are at least as predictive as those obtained from L1-norm compressive sensing. Apart from the theory, a practical implementation based on state-of-the-art mixed-integer quadratic programming (MIQP) is proposed. The robustness of our methodology is illustrated for four different transition-metal oxides with relevance as battery cathode materials: Li2xTi2(1-x)O2, Li2xNi2yO2, MgxCr2O4, and NaxCrO2. This method provides a practical and robust approach for the construction of sparser and more predictive lattice models, improving on the compressive sensing paradigm and making it applicable to a much broader range of applications.

physics.comp-ph↗

arXiv2015

Raman study of magnetic excitations and magneto-elastic coupling in alpha-SrCr2O4

Using Raman spectroscopy, we investigate the lattice phonons, magnetic excitations, and magneto-elastic coupling in the distorted triangular-lattice Heisenberg antiferromagnet alpha-SrCr2O4, which develops helical magnetic order below 43 K. Temperature dependent phonon spectra are compared to predictions from density functional theory calculations which allows us to assign the observed modes and identify weak effects arising from coupled lattice and magnetic degrees of freedom. Raman scattering associated with two-magnon excitations is observed at 20 meV and 40 meV. These energies are in general agreement with our ab-initio calculations of exchange interactions and earlier theoretical predictions of the two-magnon Raman response of triangular-lattice antiferromagnets. The temperature dependence of the two-magnon excitations indicates that spin correlations persist well above the Néel temperature.

cond-mat.str-el↗

arXiv2014

Linear magnetoelectricity at room temperature in perovskite superlattices by design

Discovering materials that display a linear magnetoelectric effect at room temperature is challenge. Such materials could facilitate novel devices based on the electric-field control of magnetism. Here we present simple, chemically intuitive design rules to identify a new class of bulk magnetoelectric materials based on the 'bicolor' layering of $Pnma$ ferrite perovskites, e.g., LaFeO$_3$/ LnFeO$_3$ superlattices for which Ln = lanthanide cation. We use first-principles density-functional theory calculations to confirm these ideas. Additionally, we elucidate the origin of this effect and show it is a general consequence of the layering of any bicolor, $Pnma$ perovskite superlattice in which the number of constituent layers are odd (leading to a form of hybrid improper ferroelectricity) and Goodenough- Kanamori rules. Here, the polar distortions induce both weak ferromagnetism and a linear magnetoelectric effect. Our calculations suggest that the effect is 2-3 times greater in magnitude than that observed for the prototypical magnetoelectric material, Cr$_2$O$_3$. We use a simple mean field model to show that the considered materials order magnetically above room temperature.

cond-mat.mtrl-sci↗

arXiv2013

Bulk magnetoelectricity in the hexagonal manganites and ferrites

Improper ferroelectricity (trimerization) in the hexagonal manganites RMnO$_3$ leads to a network of coupled structural and magnetic vortices that induce domain wall magnetoelectricity and magnetization neither of which, however, occurs in the bulk. Here we combined first-principles calculations, group-theoretic techniques, and microscopic spin models to show how the trimerization not only induces a polarization but also a bulk magnetization and bulk magnetoelectric (ME) effect. This results in the existence of a bulk linear ME vortex structure or a bulk ME coupling such that if direction of polarization reverses so does magnetization. To measure the predicted ME vortex, we suggest RMnO$_3$ under large magnetic field. We suggest a family of materials, the hexagonal RFeO$_3$ ferrites, also display the predicted phenomena in their ground state.

cond-mat.mtrl-sci↗

arXiv2012

The Magnetoelectric Effect in Transition Metal Oxides: Insights and the Rational Design of New Materials from First Principles

The search for materials displaying a large magnetoelectric effect has occupied researchers for many decades. The rewards could include not only advanced electronics technologies, but also fundamental insights concerning the dielectric and magnetic properties of condensed matter. In this article, we focus on the magnetoelectric effect in transition metal oxides and review the manner in which first-principles calculations have helped guide the search for (and increasingly, predicted) new materials and shed light on the microscopic mechanisms responsible for magnetoelectric phenomena.

cond-mat.mtrl-sci↗

arXiv2011

RbFe2+Fe3+F6: Synthesis, Structure, and Characterization of a New Charge-Ordered Magnetically Frustrated Pyrochlore-Related Mixed-Metal Fluoride

A new charge-ordered magnetically frustrated mixed-metal fluoride with a pyrochlore-related structure has been synthesized and characterized. The material, RbFe2F6 (RbFe2+Fe3+F6) was synthesized through mild hydrothermal conditions. The material exhibits a three-dimensional pyrochlore-related structure consisting of corner-shared Fe2+F6 and Fe3+F6 octahedra. In addition to single crystal diffraction data, neutron powder diffraction and magnetometry measurements were carried out. Magnetic data clearly reveal strong antiferromagnetic interactions (a Curie-Weiss temperature of -270 K) but sufficient frustration to prevent ordering until 16 K. No structural phase transformation is detected from the variable temperature neutron diffraction data. Infrared, UV -vis, thermogravimetric, and differential thermal analysis measurements were also performed. First-principles density functional theory (DFT) electronic structure calculations were also done. Crystal data: RbFe2F6, orthorhombic, space group Pnma (No. 62), a = 7.0177(6) Å, b = 7.4499(6) Å, c = 10.1765(8) Å, V = 532.04(8) Å3, Z = 4.

cond-mat.mtrl-sci↗

arXiv2011

Size control of Charge-Orbital Order in Half-Doped Manganite, La$_{0.5}$Ca$_{0.5}$MnO$_3$

Motivated by recent experimental results, we study the effect of size reduction on half-doped manganite, La$_{0.5}$Ca$_{0.5}$MnO$_3$, using the combination of density functional theory (DFT) and dynamical mean field theory (DMFT). We find that upon size reduction, the charge-ordered antiferromagnetic phase, observed in bulk, to be destabilized, giving rise to the stability of a ferromagnetic metallic state. Our theoretical results, carried out on defect-free nanocluster in isolation, establish the structural changes that follow upon size reduction to be responsible for this. Our study further points out the effect of size reduction to be distinctively different from application of hydrostatic pressure. Interestingly, our DFT+DMFT study, additionally, reports the correlation-driven stability of charge-orbitally ordered state in bulk La$_{0.5}$Ca$_{0.5}$MnO$_3$, even in absence of long range magnetic order.

cond-mat.str-el↗

arXiv2011

Multi-step approach to microscopic models for frustrated quantum magnets - the case of the natural mineral azurite

The natural mineral azurite Cu$_3$(CO$_3$)$_2$(OH)$_2$ is a frustrated magnet displaying unusual and controversially discussed magnetic behavior. Motivated by the lack of a unified description for this system, we perform a theoretical study based on density functional theory as well as state-of-the-art numerical many-body calculations. We propose an effective generalized spin-1/2 diamond chain model which provides a consistent description of experiments: low-temperature magnetization, inelastic neutron scattering, nuclear magnetic resonance measurements, magnetic susceptibility as well as new specific heat measurements. With this study we demonstrate that the balanced combination of first principles with powerful many-body methods successfully describes the behavior of this frustrated material.

cond-mat.str-el↗

arXiv2011

Origin of Magnetism and trend in $T_{c}$ in Cr-based double perovskites: Interplay of two driving mechanisms

Employing first principles density functional calculations, together with solution of the low-energy, model Hamiltonian constructed in a first principles manner, we explored the origin of magnetism and $T_c$ trend in Cr-based double perovskite series, Sr$_2$CrB$'$O$_6$ (B$'$=W/Re/Os). Our study shows that the apparently puzzling $T_c$ trend in Sr$_2$CrB$'$O$_6$ (B$'$=W/Re/Os) series can be understood in terms of the interplay of the hybridization driven mechanism and the super-exchange mechanism.

cond-mat.mtrl-sci↗

arXiv2010

Piezoelectrics by Design: A Route through Short-period Perovskite Superlattices

Using first-principles density functional theory, we study piezoelectricity in short-period superlattices made with combination of ferroelectric and paraelectric components and exhibiting polar discontinuities. We show that piezoelectric response of such a superlattice can be tuned both in terms of sign and magnitude with a choice of its components. As these superlattices with nonswitchable polarization do not undergo ferroelectric transitions, we predict them to exhibit a robust piezoelectric response with weaker temperature dependence compared to their bulk counterparts.

physics.comp-ph↗

arXiv2010

Chemical control of polar behavior in bicomponent short-period superlattices

Using first-principles density functional calculations, we study the interplay of ferroelectricity and polar discontinuities in a range of 1-1 oxide superlattices, built out of ferroelectric and paraelectric components. Studies have been carried out for a varied choice of chemical composition of the components. We find that, when polar interfaces are present, the polar discontinuities induce off- centric movements in the ferroelectric layers, even though the ferroelectric is only one unit cell thick. The distortions yield non-switchable polarizations, with magnitudes comparable to those of the corresponding bulk ferroelectrics. In contrast, in superlattices with no polar discontinuity at the interfaces, the off-centric movements in the ferroelectric layer are usually suppressed. The details of the behavior and functional properties are, however, found to be sensitive to epitaxial strain, rotational instabilities and second-order Jahn-Teller activity, and are therefore strongly in uenced by the chemical composition of the paraelectric layer.

physics.comp-ph↗

arXiv2009

Evidence of Kinetic Energy Driven Antiferromagnetism in Double Perovskites : A First-principles Study

Using first principles density functional calculations, together with exact diagonalization of Fe-Mo Hamiltonian constructed in a first principles Wannier function basis, we studied the electronic structure of La doped double perovskite compound Sr$_2$FeMoO$_6$. Our calculation show stabilization of kinetic energy driven antiferromagnetic phase for La rich compounds, in agreement with the results obtained on the basis of previous model calculations.

cond-mat.mtrl-sci↗

arXiv2008

Electronic Structure, Phonons and Dielectric Anomaly in Ferromagnetic Insulating Double Perovskite La2NiMnO6

Using first-principles density functional calculations, we study the electronic and magnetic properties of ferromagnetic insulating double-perovskite compound La2NiMnO6, which has been reported to exhibit interesting magnetic field sensitive dielectric anomaly as a function of temperature. Our study reveals existence of very soft infra-red active phonons that couple strongly with spins at the Ni and Mn sites through modification of the super-exchange interaction. We suggest that these modes are the origin for observed dielectric anomaly in La2NiMnO6.

cond-mat.mtrl-sci↗