arXiv subjects

S. D. Kaushik

Publications and source records attributed to S. D. Kaushik.

At least 19 recordsLinked to original sources

arXiv2026

Ultra-Soft Ferrimagnetism in a High-Entropy Spinel Oxide Driven by Site-Selective Cation Disorder

High-entropy materials are complex, multifunctional materials that have reshaped the design of advanced functional materials. Their chemically diverse compositions enable access to a broader compositional space than conventional solid solutions, while simultaneously posing significant challenges for fundamental structure property understanding. In this study, we introduce a new highentropy spinel oxide with an exceptionally low coercivity of 1.8 Oe at room temperature, among the lowest reported for bulk spinel oxides, and a high electrical resistivity (1560 ohm-cm). Neutron powder diffraction (NPD) and magnetic measurements reveal long-range collinear ferrimagnetic ordering (k = 0,0,0) with a transition temperature at 420 K. This rare combination of ultra-soft magnetic behavior, robust ferrimagnetic ordering well above room temperature, and high resistivity highlights its strong potential as an advanced soft-magnetic oxide for low-loss, high-frequency applications. Furthermore, X-ray absorption spectroscopy (XAS), Mossbauer spectroscopy, and NPD analyses were combined to determine the cation distribution and site selectivity across the tetrahedral and octahedral sites of the complex structure.

cond-mat.mtrl-sci↗

arXiv2026

Long-range magnetic ordering and structural phase transition in disordered high-entropy spinel chromites

High-entropy spinel oxides provide an excellent platform for investigating entropy-stabilized correlated systems with strong configurational disorder. In this work, we systematically study the temperature evolution of the structural and magnetic properties of Cr-based high-entropy spinels with compositions $(Mn_{0.2}Co_{0.2}Ni_{0.2}Cu_{0.2}Zn_{0.2})Cr_2O_4$ and $(Mg_{0.2}Co_{0.2}Ni_{0.2}Cu_{0.2}Zn_{0.2})Cr_2O_4$. Our results reveal that both systems crystallize in cubic structure with space group \textit{$Fd\overline{3}m$} at room temperature. Each system undergoes antiferromagnetic ordering below the Néel temperatures $ T_N$ = 49 K and 35 K, respectively. Neutron diffraction measurements confirm the emergence of long-range magnetic order with spiral spin arrangement. Both systems exhibit a structural phase transition from cubic \textit{$Fd\overline{3}m$} to orthorhombic \textit{Fddd} symmetry at approximately 55 K and 85 K, respectively. Notably, despite the significant chemical disorder at the A site, both systems undergo transitions analogous to those observed in low entropy spinel systems. This behavior suggests that high configurational entropy may promote global structural stabilization despite local chemical disorder, thereby preserving long-range orderings and the characteristic symmetry-breaking transitions of the pristine spinel systems.

cond-mat.mtrl-sci↗

arXiv2026

Coupled phase transitions in crystalline solids with extreme chemical disorder

Structural phase transitions often couple to magnetic and electronic degrees of freedom, enabling emergent phenomena in solids. In high-entropy oxides (HEOs), which typically stabilize in highly symmetric cubic phases, such transitions are considered rare due to the extreme chemical disorder-analogous to the behavior observed in high-entropy alloys. This raises a fundamental question: can the rich physics of coupled phase transitions persist in such disordered systems? Here, we show that targeted design of compositionally complex oxides (CCOs) can trigger symmetry-lowering transitions, with spinel-type materials serving as a representative case. For instance, [Mn$_{0.2}$Co$_{0.2}$Ni$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$]Cr$_2$O$_4$, having two Jahn-Teller (J-T) active ions, undergoes two successive coupled structural transitions upon cooling: an orbital-driven transition at 100 K and a magnetism-driven transition at 40 K. Systematic substitution of $A$-site cations reveals that both Ni and Cu are essential for these transitions. Element specific local structure investigations uncover distinct and opposing local distortions around Ni and Cu, while Mn, Co, and Zn remain largely undistorted. These results establish that CCOs can host coupled phase transitions through `cooperation via competition' among local distortions in a chemically disordered lattice. This discovery expands the design principles for complex oxides, introducing a new paradigm for tuning structural and functional properties in high-entropy systems beyond conventional symmetry constraints.

cond-mat.mtrl-sci↗

arXiv2025

Investigating structure and physical properties of quaternary layered transition metal oxide Na2Cu2TeO6

We investigated the crystal structure, magnetic behavior, and optical properties of the layered honeycomb compound Na2Cu2TeO6. X-ray and neutron diffraction confirmed a monoclinic structure, with Cu ions arranged in dimerized chains. Magnetic susceptibility measurements yielded a Curie-Weiss temperature significantly lower than the expected spin-only value, indicating the presence of strong antiferromagnetic interactions and enhanced quantum fluctuations. A broad maximum near 160 K in the susceptibility data is consistent with short-range one-dimensional antiferromagnetic correlations. Magnetization measurements showed negligible coercivity, and specific heat data revealed no anomalies down to 3 K. Temperature-dependent neutron diffraction showed no evidence of long-range magnetic order. Optical absorption studies using UV-Visible spectroscopy displayed a sharp absorption edge in the UV region. Tauc analysis estimated a direct optical band gap of approximately 2.10 eV, with no clear indication of an indirect transition. These observations provide insight into the interplay between structural distortions, low-dimensional magnetism, and optical behavior in Na2Cu2TeO6

cond-mat.str-el↗

arXiv2025

Local structural distortions drive magnetic molecular field in compositionally complex spinel oxide

Understanding how local distortions determine the functional properties of high entropy materials, containing five or more elements at a crystallographic site, is an open challenge. We address this for a compositionally complex spinel oxide (Mn$_{0.2}$Co$_{0.2}$Ni$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$)Cr$_2$O$_4$ ($A^5$Cr$_2$O$_4$). By comparatively examining extended X-ray absorption fine structure on $A^5$Cr$_2$O$_4$ and its parent counterparts $A$Cr$_2$O$_4$ along with density functional theory calculations for multiple configurations, we find that the element-specific distortions go beyond the first neighbor. Specifically, the strong Jahn-Teller distortion present in CuCr$_2$O$_4$ is found to be completely suppressed in $A^5$Cr$_2$O$_4$. Instead, there is a broad distribution of Cu-O and Cu-Cr bond distances while other $A$-O distances acquire certain specific values. This study demonstrates the additional flexibility of a cationic sublattice in maintaining a uniform long-range structure, in contrast to previous reports showing only the accommodative anionic sublattice. Remarkably, despite the presence of multiple magnetic ions and variable bond lengths, the mean field magnetic interactions of $A^5$Cr$_2$O$_4$ exhibit a striking resemblance to those of NiCr$_2$O$_4$. This compelling observation originates from the comparability of bond lengths around Cr in both materials. Our study paves the way for a deeper understanding of the impact of local structural distortions in compositionally complex quantum materials, enabling the targeted design with tailored properties.

cond-mat.mtrl-sci↗

arXiv2024

Validating Mean Field Theory in a New Complex, Disordered High-Entropy Spinel Oxide

The advent of novel high-entropy oxides has sparked substantial research interest due to their exceptional functional properties, which often surpass the mere sum of their constituent elements' characteristics. This study introduces a complex high-entropy spinel oxide with composition (Ni$_{0.2}$Mg$_{0.2}$Co$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$)(Mn$_{0.66}$Fe$_{0.66}$Cr$_{0.66}$)O$_{4}$. We performed comprehensive structural (X-ray and Neutron diffraction), microstructural, magnetic, and local electronic structure investigations on this material. Despite the material's high degree of disorder, detailed magnetization measurements and low temperature neutron powder diffraction studies reveal long-range ferrimagnetic ordering beginning at 293 K. The sample exhibits a high saturation magnetization of 766 emu-cm${^3}$ (at 50 K), a low coercivity (H$_C$) of 100 Oe (50 K), a high transition temperature (T$_C$) around room temperature, and high resistivity value of 4000 Ohm-cm at room temperature, indicating its potential for high density memory devices. The magnetic structure is determined using a collinear-type ferrimagnetic model with a propagation vector k = 0,0,0. Various analytical techniques, including modified Arrott plots, Kouvel-Fischer analysis, and critical isotherm analysis, are employed to investigate the phase transitions and magnetic properties of this complex system. Our results indicate a second-order phase transition. Remarkably, despite the complex structure and significant disorder, the critical exponents obtained are consistent with the mean field model. The high entropy leads to a remarkably homogeneous distribution of multiple cations, validating the approximation of average local magnetic environments and supporting the mean field theory.

cond-mat.str-el↗

arXiv2024

Enhanced metamagnetic shape memory effect in Heusler-type Ni37Co11Mn43Sn9 polycrystalline ferromagnetic shape memory alloy

Polycrystalline Ni-Co-Mn-Sn based ferromagnetic shape memory alloys (FSMAs) show promise as actuator materials, but their practical application involving magnetic field induced strain (MFIS) is often limited by three factors: the requirement for high magnetic fields (> 5 T), martensitic transition temperature away from room temperature, and limited recovery of pre-strain applied to the martensite phase. Current work investigates the martensitic transition (MT) and shape memory effect under the application of magnetic field for bulk polycrystalline Ni37Co11Mn43Sn9 alloy. The outcome of the study reveals a metamagnetic transition from the martensitic phase to the austenitic phase at a low field of 2.8 T at 300 K which results 0.25% spontaneous MFIS. Interestingly, 1.3% pre-strained specimen registers a 100% recovery with the application of magnetic field of 4.5 T. Furthermore, the pre-strained specimen exhibited a two-way shape memory effect between a strain value of 1.0% to 1.55% during the field loading and unloading sequences. Notably, this study also demonstrates, to the best of our knowledge , for the first time, that the spontaneous strain and pre-strain add together. This finding paves the way for achieving a giant MFIS by pre-straining a Ni-Mn-Sn/In class of FSMAs which shows large spontaneous MFIS.

cond-mat.mtrl-sci↗

arXiv2021

Nonmonotonic magnetic field dependence of remanent ferroelectric polarization in reduced-graphene-oxide-BiFeO$_3$ nanocomposite

In a nanocomposite of reduced graphene oxide (RGO) and BiFeO$_3$ (BFO), the remanent ferroelectric polarization is found to follow nonmonotonic magnetic field dependence at room temperature as the applied magnetic field is swept across 0-20 kOe on a pristine sample. The remanent ferroelectric polarization is determined both from direct electrical measurements on an assembly of nanoparticles and powder neutron diffraction patterns recorded under 0-20 kOe field. The nanosized ($\sim$20 nm) particles of BFO are anchored onto the graphene sheets of RGO via Fe-C bonds with concomitant rise in covalency in the Fe-O bonds. The field-dependent competition between the positive and negative magnetoelectric coupling arising from magnetostriction due to, respectively, interface and bulk magnetization appears to be giving rise to the observed nonmonotonic field dependence of polarization. The emergence of Fe-C bonds and consequent change in the magnetic and electronic structure of the interface region has influenced the coupling between ferroelectric and magnetic properties remarkably and thus creates a new way of tuning the magnetoelectric properties via reconstruction of interfaces in nanocomposites or heterostructures of graphene/single-phase-multiferroic systems.

cond-mat.mtrl-sci↗

arXiv2021

Investigation of spin-phonon coupling and local magnetic properties in magnetoelectric Fe2TeO6

Spin-phonon coupling originated from spin-lattice correlation depends upon different exchange interactions in transition metal oxides containing 3d magnetic ions. Spin-lattice coupling can influence the coupling mechanism in magnetoelectric material. To understand the spin-lattice correlation in inverse trirutile Fe2TeO6 (FTO), magnetic properties and phonon spectra are studied. Signature of short-range magnetic correlation induced by 5/2-5/2 dimeric interaction and magnetic anomaly at 150 K is perceived apart from the familiar sharp transition (TN~210K) corresponding to long-range order by magnetization and heat capacity measurement. The magnetic transitions and the spin dynamics are further locally probed by muon spin resonance (μSR) measurement in both zero fields (ZF) and longitudinal field (LF) mode. Three dynamically distinct temperature regimes; (i) T >TN, (ii) TN>T>150 K, and (iii) T<150 K, are observed. A swift change in spin dynamics is realized at 150K by μSR, though previous studies suggest long-range antiferromagnetic order. The observation of renormalization of different Raman modes below 210K suggests the existence of spin-phonon coupling in the material. The coupling strength is quantified as in the range 0.1-1.2 cm-1 following the two-spin cluster approximation. We propose that the spin-phonon coupling is mediated by the Fe-O2-Fe interbilayer exchange play a significant role in ME coupling observed in the material.

cond-mat.str-el↗

arXiv2021

d5-off-centering induced ferroelectric and magnetoelectric correlations in trirutile-Fe2TeO6

We present the rare existence of d5 off-centering, weak ferroelectric polarization and demonstrate its correlation with observed magnetoelectric (ME) properties in the G type (TN~210 K) antiferromagnet Fe2TeO6 (FTO) compound. The origin of ferroelectricity (FE) is associated with both lattice and asymmetric electron density distribution around the ion cores. ME coupling is observed in magnetic field-dependent polarization, ME voltage, and magnetostrain measurements. Short-range magnetic ordering due to intrabilayer dimeric exchange coupling via the double oxygen bridged Fe-O1-Fe pathway is proposed to play a dominating role to exhibit the negative nonlinear magnetic field dependent ME behavior at 300 K. Interbilayer exchange via Fe-O2-Fe pathways dominantly determines the hysteretic nonlinear magnetic field dependent ME response below TN. The observed nonlinear ME coupling signifies magnetoelasticity as manifested in the temperature and magnetic field-dependent strain measurement. Hence the rare existence of ferroelectricity and magnetoelectric coupling by d5 ion is presented in FTO.

cond-mat.mtrl-sci↗

arXiv2020

Crossover from meta-magnetic state to spin-glass behaviour upon Ti-substitution for Mn in CuMn2O4

Tetragonal distorted spinel of CuMn2-xTixO4 (x = 0, 0.25 and 0.50) was prepared by solid state reaction method followed by neutron diffraction, FTIR spectroscopy, dielectric spectroscopy and magnetization measurements. The neutron diffraction and FTIR spectroscopy provide the information regarding phase formation. But, the magnetic susceptibility clearly shows the ferri-magnetic order below 76K associated with meta-magnetic state which turns to spin-glass behaviour upon Ti-substitution for Mn in CuMn2O4. In addition, the room temperature M(H) of all the spinels are described by the Arrott's plot for weak ferromagnetism. Further, the room temperature dielectric measurement provides the electronic property of CuMn2O4 dominated by grain boundary effect that is significantly increased upon Ti-substitution for Mn in CuMn2O4.

cond-mat.mtrl-sci↗

arXiv2020

Oxygen vacancy induced electronic structure modification of KTaO$_3$

The observation of metallic interface between band insulators LaAlO$_3$ and SrTiO$_3$ has led to massive efforts to understand the origin of the phenomenon as well as to search for other systems hosting such two dimensional electron gases (2-DEG). However, the understanding of the origin of the 2-DEG is very often hindered as several possible mechanisms such as polar catastrophe, cationic intermixing and oxygen vacancy (OV) etc. can be operative simultaneously. The presence of a heavy element makes KTaO$_3$ (KTO) based 2-DEG a potential platform to investigate spin orbit coupling driven novel electronic and magnetic phenomena. In this work, we investigate the sole effect of the OV, which makes KTO metallic. Our detailed \textit{ab initio} calculations not only find partially filled conduction bands in the presence of an OV but also predict a highly localized mid-gap state due to the linear clustering of OVs around Ta. Photoluminescence measurements indeed reveal the existence of such mid-gap state and O $K$-edge X-ray absorption spectroscopy finds electron doping in Ta $t_{2g}^*$ antibonding states. This present work suggests that one should be cautious about the possible presence of OVs within KTO substrate in interpreting metallic behavior of KTO based 2-DEG.

cond-mat.mtrl-sci↗

arXiv2019

Origin of Ferroelectricity in Orthorhombic LuFeO$_3$

We demonstrate that small but finite ferroelectric polarization ($\sim$0.01 $μ$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.

cond-mat.str-el↗

arXiv2019

Magnetic ordering of the martensite phase in Ni-Co-Mn-Sn-based ferromagnetic shape memory alloys

The magnetic state of low temperature martensite phase in Co-substituted Ni-Mn-Sn-based ferromagnetic shape memory alloys (FSMAs) has been investigated, in view of numerous conflicting reports of occurrences of spin glass (SG), superparamagnetism (SPM) or long range anti-ferromagnetic (AF) ordering. Combination of dc magnetization, ac susceptibility and small angle neutron scattering (SANS) studies provide a clear evidence for AF order in martensitic phase of Ni45Co5Mn38Sn12 alloy and rule out SPM and SG orders. Identical studies on another alloy of close composition of Ni44Co6Mn40Sn10 point to presence of SG order in martensitic phase and absence of SPM behavior, contrary to earlier report. SANS results do show presence of nanometre-sized clusters but they are found to grow in size from 3 nm at 30 K to 11 nm at 300 K, and do not correlate with magnetism in these alloys.

cond-mat.mtrl-sci↗

arXiv2018

Origin of magnetic moments and presence of a resonating valence bond state in Ba$_2$YIrO$_6$

While it was speculated that 5$d^4$ systems would possess non-magnetic $J$~=~0 ground state due to strong Spin-Orbit Coupling (SOC), all such systems have invariably shown presence of magnetic moments so far. A puzzling case is that of Ba$_2$YIrO$_6$, which in spite of having a perfectly cubic structure with largely separated Ir$^{5+}$ ($d^4$) ions, has consistently shown presence of weak magnetic moments. Moreover, we clearly show from Muon Spin Relaxation ($μ$SR) measurements that a change in the magnetic environment of the implanted muons in Ba$_2$YIrO$_6$ occurs as temperature is lowered below 10~K. This observation becomes counterintuitive, as the estimated value of SOC obtained by fitting the RIXS spectrum of Ba$_2$YIrO$_6$ with an atomic $j-j$ model is found to be as high as 0.39~eV, meaning that the system within this model is neither expected to possess moments nor exhibit temperature dependent magnetic response. Therefore we argue that the atomic $j-j$ coupling description is not sufficient to explain the ground state of such systems, where despite having strong SOC, presence of hopping triggers delocalisation of holes, resulting in spontaneous generation of magnetic moments. Our theoretical calculations further indicate that these moments favour formation of spin-orbital singlets in the case of Ba$_2$YIrO$_6$, which is manifested in $μ$SR experiments measured down to 60~mK.

cond-mat.mtrl-sci↗

arXiv2018

Nonmonotonic particle-size-dependence of magnetoelectric coupling in strained nanosized particles of BiFeO$_3$

Using high resolution powder x-ray and neutron diffraction experiments, we determined the off-centered displacement of the ions within a unit cell and magnetoelectric coupling in nanoscale BiFeO$_3$ ($\approx$20-200 nm). We found that both the off-centered displacement of the ions and magnetoelectric coupling exhibit nonmonotonic variation with particle size. They increase as the particle size reduces from bulk and reach maximum around 30 nm. With further decrease in particle size, they decrease precipitously. The magnetoelectric coupling is determined by the anomaly in off-centering of ions around the magnetic transition temperature ($T_N$). The ions, in fact, exhibit large anomalous displacement around the $T_N$ which is analyzed using group theoretical approach. It underlies the nonmonotonic particle-size-dependence of off-centre displacement of ions and magnetoelectric coupling. The nonmonotonic variation of magnetoelectric coupling with particle size is further verified by direct electrical measurement of remanent ferroelectric hysteresis loops at room temperature under zero and $\sim$20 kOe magnetic field. Competition between enhanced lattice strain and compressive pressure appears to be causing the nonmonotonic particle-size-dependence of off-centre displacement while coupling between piezo and magnetostriction leads to nonmonotonicity in the variation of magnetoelectric coupling.

cond-mat.mtrl-sci↗

arXiv2018

Evidence for two spin-glass transitions with magnetoelastic and magnetoelectric couplings in the multiferroic (Bi$_{1-x}$Ba$_x$)(Fe$_{1-x}$Ti$_x$)O$_3$ system

For disordered Heisenberg systems with small single ion anisotropy, two spin glass transitions below the long range ordered phase transition temperature has been predicted theoretically for compositions close to the percolation threshold. Experimental verification of these predictions is still controversial for conventional spin glasses. We show that multiferroic spin glass systems can provide a unique platform for verifying these theoretical predictions via a study of change in magnetoelastic and magnetoelectric couplings, obtained from an analysis of diffraction data, at the spin glass transition temperatures. Results of macroscopic and microscopic (x-ray and neutron scattering) measurements are presented on disordered BiFeO3, a canonical Heisenberg system with small single ion anisotropy, which reveal appearance of two spin glass phases SG1 and SG2 in coexistence with the LRO phase below the A-T and G-T lines. It is shown that the temperature dependence of the integrated intensity of the antiferromagnetic peak shows dips with respect to the Brillouin function behaviour around the SG1 and SG2 transition temperatures. The ferroelectric polarisation changes significantly at the two spin glass transition temperatures. These results, obtained using microscopic techniques, clearly demonstrate that the SG1 and SG2 transitions occur on the same magnetic sublattice and are intrinsic to the system. We also construct a phase diagram showing all the magnetic phases in BF-xBT system. While our results on the two spin glass transitions support the theoretical predictions, it also raises several open questions which need to be addressed by revisiting the existing theories of spin glass transitions by taking into account the effect of magnetoelastic and magnetoelectric couplings as well as electromagnons.

cond-mat.mtrl-sci↗

arXiv2017

Cobalt substitution induced magnetodielectric enhancement in multiferroic Bi2Fe4O9

Antiferromagnetic Bi_{2}Fe_{4}O_{9} (BFO), lightly substituted by cobalt is studied for magnetodielectricity. The substitution causes a substantial decrease in the Neel temperature (T_N) from 250 K (in parent sample, BFO) to 152 K (in 2% Co substituted sample). At the same time, the substituted samples display a pronounced irreversibility in the ZFC-FC magnetization data for T $<$ 370 K and opening of hysteresis in the M-H plot, thus signifying the onset of weak ferromagnetism (FM) and magnetic glassiness. The induced magnetic glassiness is found to slow down the dynamics such that the magnetization decay follows. The dielectric measurement in the same temperature window shows unusual oppression in, for T$\sim$T_N and contrasting nature of tan loss for temperatures above and below T_N, thus hinting a plausible coupling between the magnetic and electric order parameters. A confirmation to this coupling is seen in the magnetodielectric (MD) results, in which it is found that the substitution induces an additional component in the MD, apart from the usual components in BFO. This additional component of MD is found to obey behaviour, with the n values being comparable to 1-p of magnetization. The temperature variation of MD also shows a contrasting behaviour for the parent and 2% Co substituted sample with an enhancement of two times in MD value. In summary, our study shows ME coupling introduced by the magnetic glassiness and its behaviour is very much different from the intrinsic one.

cond-mat.mtrl-sci↗