arXiv subjects

V. Siruguri

Publications and source records attributed to V. Siruguri.

At least 19 recordsLinked to original sources

arXiv2023

Magnetic-field induced melting of long-range magnetic order akin to Kitaev insulators in the metallic compound Tb5Si3

There have been constant efforts to find exotic quantum spin-liquid (QSL) materials. Some of the transition metal insulators dominated by the direction dependent anisotropic exchange interaction (Kitaev model for honeycomb network of magnetic ions) are considered to be promising cases for the same. In such Kitaev insulators, QSL is achieved from the zero-field antiferromagnetic state by the application of magnetic field, suppressing other exchange interactions responsible for magnetic order. Here, we show that the features attributable to long-range magnetic ordering of the intermetallic compound, Tb5Si3 (T_N= 69 K), containing honey-comb network of Tb ions, are completely suppressed by a critical applied field, H_cr, in heat-capacity and magnetization data, mimicking the behavior of Kitaev physics candidates. The neutron diffraction patterns as a function of H reveal that it is an incommensurate magnetic structure that gets suppressed, showing peaks arising from multiple wave vectors beyond Hcr. Increasing magnetic entropy as a function of H with a peak in the magnetically ordered state is in support of some kind of magnetic disorder in a narrow field range after H_cr. Such a high-field behavior for a metallic heavy rare-earth system to our knowledge has not been reported in the past and therefore is intriguing.

cond-mat.str-el↗

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

Unusual spin dynamics in the low-temperature magnetically ordered state of Ag$_{3}$LiIr$_{2}$O$_{6}$

Recently, there have been contrary claims of Kitaev spin-liquid behaviour and ordered behavior in the honeycomb compound Ag$_3$LiIr$_2$O$_6$ based on various experimental signatures. Our investigations on this system reveal a low-temperature ordered state with persistent dynamics down to the lowest temperatures. Magnetic order is confirmed by clear oscillations in the muon spin relaxation ($μ$SR) time spectrum below 9 K till 52 mK. Coincidentally in $^7$Li nuclear magnetic resonance, a wipe-out of the signal is observed below $\sim$ 10 K which again strongly indicates magnetic order in the low temperature regime. This is supported by our density functional theory calculations which show an appreciable Heisenberg exchange term in the spin Hamiltonian that favors magnetic ordering. The $^7$Li shift and spin-lattice relaxation rate also show anomalies at $\sim$ 50 K. They are likely related to the onset of dynamic magnetic correlations, but their origin is not completely clear. Detailed analysis of our $μ$SR data is consistent with a co-existence of incommensurate Néel and striped environments. A significant and undiminished dynamical relaxation rate ($\sim 5$ MHz) as seen in $μ$SR deep into the ordered phase indicates enhanced quantum fluctuations in the ordered state.

cond-mat.str-el↗

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↗

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

Spin reorientation and disordered rare earth magnetism in Ho$_2$FeCoO$_6$

We report the experimental observation of spin reorientation in the double perovskite Ho$_2$FeCoO$_6$. The magnetic phase transitions in this compound are characterized and studied through magnetization and specific heat, and the magnetic structures are elucidated by neutron powder diffraction. Two magnetic phase transitions are observed in this compound - one at $T_\mathrm{N1} \approx$ 250~K, from paramagnetic to antiferromagnetic, and the other at $T_\mathrm{N2} \approx$ 45~K, from a phase with mixed magnetic structures to a single phase through a spin reorientation process. The magnetic structure in the temperature range 200~K - 45~K is a mixed phase of the irreducible representations $Γ_1$ and $Γ_3$, both of which are antiferromagnetic. The phase with mixed magnetic structures that exists in Ho$_2$FeCoO$_6$ gives rise to a large thermal hysteresis in magnetization that extends from 200~K down to the spin reorientation temperature. At $T_\mathrm{N2}$, the magnetic structure transforms to $Γ_1$. Though long-range magnetic order is established in the transition metal lattice, it is seen that only short-range magnetic order prevails in Ho$^{3+}$ - lattice. Our results should motivate further detailed studies on single crystals in order to explore spin reorientation process, spin switching and the possibility of anisotropic magnetic interactions giving rise to electric polarization in Ho$_2$FeCoO$_6$.

cond-mat.mtrl-sci↗

arXiv2017

Disorder-Driven Spin-Reorientation in Multiferroic $h-YMn_{1-x}Fe_xO_3$

Magnetic structure evolution of multiferroic hexagonal $YMn_{1-x}Fe_{x}O_{3}$ (${x} = 0, 0.05,$ and $0.1$) has been studied by carrying out detailed temperature-dependent neutron diffraction at zero- and 5T-fields. Thermodynamic data confirm antiferromagnetic ordering at $T_{N}$ in all the compositions. Our sub-$T_{N}$ neutron diffraction results assign the magnetic structure of pure $YMnO_3$ to $Γ_{1}$ irreducible representation. Over the perturbative-doping range, the magnetic configuration changes via $Γ_{1}+Γ_{2}$ for $YMn_{0.95}Fe_{0.05}O_{3}$ on to $Γ_{2}$ for $YMn_{0.9}Fe_{0.1}O_{3}$, as the maiden compositional analogue of spin-reorientation; its occurrence in temperature-domain already reported for several manganites. Moreover, while the large thermal isostructural changes observed above ${T}_{N}$ are subdued in the ordered state, small alterations by the applied 5T-field are relatively uniform across, confirming strong magneto-elastic nature of the system. Decrease of the ordered magnetic moment ($μ_{ord}$) and planar magnetic frustration noted with Fe-doping is enhanced by the applied field, apparently through canting.

cond-mat.mtrl-sci↗

arXiv2017

Effect of Frustrated Exchange Interactions and Spin-half Impurity on the Electronic Structure of Strongly Correlated NiFe$_{2}$O$_{4}$

Spin-polarized density functional calculations, magnetization, and neutron diffraction measurements are carried out to investigate the magnetic exchange interactions and strong correlation effects in Yb substituted inverse spinel nickel ferrite. In the pristine form, the compound is found to be a mixed insulator under the Zaanen-Sawtazsky-Allen classification scheme as it features both charge transfer and Mott insulator mechanism. Estimation of magnetic exchange couplings reveals that both octahedral-octahedral and octahedral-tetrahedral spin-spin interactions are antiferromagnetic which is typical of a spin-frustrated triangular lattice. However, the latter is dominant compared to the former leading to a forced parallel alignment of the spins at the octahedral site which is in agreement with the results of neutron diffraction measurements. The substituent Yb is found to be settled in +3 charge state, as confirmed from the XPS measurements, to behave like a spin-half impurity carried by the localized $f_{z(x^2-y^2)}$ orbital. The impurity $f$ spin significantly weakens the antiferromagnetic coupling with the spins at the tetrahedral site, which explains the experimental observation of fall in Curie temperature with Yb substitution.

cond-mat.mtrl-sci↗

arXiv2017

Re-entrant spin-glass freezing and magneto-dielectric behavior of Li3NiRuO6, a layered rock-salt related oxide

We report the results of neutron diffraction, ac and dc magnetization, heat-capacity, complex permittivity, and pyrocurrent measurements on an oxide, Li3NiRuO5, hitherto not paid much attention in the literature, except for a previous report on its promising electrochemical performance. We emphasize on the following findings: (i) Observation of re-entrant spin-glass behavior; that is, this oxide undergoes ferrilmagnetic ordering below 8- K, entering spin-glass regime around 12 K. (ii) There is no prominent feature in the complex dielectric permittivity (in particular, at the magnetic transitions) in the absence of external magnetic field, indicative of the absence of ferroelectricity. However, there is a distinct evidence for magneto-dielectric (MDE) coupling. The sign of MDE coupling also changes as the sample is cooled from ferrimagnetic state to spin-glass regime. (iii) There are pyroelectric anomalies in the vicinity of 30-70 K, presumably from thermally stimulated depolarization current.

cond-mat.str-el↗

arXiv2016

Correlation of exchange bias with magneto-structural effects across the compensation temperature of Co(Cr$_{1-x}$Fe$_{x}$)$_2$O$_4$ (x = 0.05 and 0.075)

A small amount of Fe (5% and 7.5%) substitution in the Cr-site of the multiferroic compound CoCr2O4 leads to a magnetization reversal. In these compounds, we report a sign change in the exchange bias across the compensation temperature, accompanied by a non-monotonic change in the local moments across the compensation temperature. Such non-monotonic change in the magnetic moments is triggered by a similar change in the lattice structure. We relate here the sign change of exchange bias with that of the crystalline energy of the lattice and the Zeeman energy term arising from the anti-site disorder.

cond-mat.str-el↗

arXiv2015

Novel thermal effects across first order magnetic transition in Ta doped $HfFe_2$ intermetallic

Novel thermal effects across the first order antiferromagnetic (AFM) - ferromagnetic (FM) transition in an intermetallic alloy are reported. They show instances of warming when heat is extracted from the sample, and cooling when heat is provided to the sample across AFM-FM transition in Ta doped $HfFe_2$, thus providing indisputable evidence of metastable supercooled AFM and superheated FM states, respectively. Such thermal effects in a magnetic solid prepared from commercially available materials has been reported for the first time. The transition proceeds in multiple steps which is interpreted in the framework of quenched disorder broadening of AFM-FM transition and classical nucleation theory. Measurements in the presence of magnetic field conform to above frame work.

cond-mat.str-el↗

arXiv2014

Large magnetoelectric coupling in nanoscale BiFeO$_3$ from direct electrical measurements

We report the results of direct measurement of remanent hysteresis loops on nanochains of BiFeO$_3$ at room temperature under zero and $\sim$20 kOe magnetic field. We noticed a suppression of remanent polarization by nearly $\sim$40\% under the magnetic field. The powder neutron diffraction data reveal significant ion displacements under a magnetic field which seems to be the origin of the suppression of polarization. The isolated nanoparticles, comprising the chains, exhibit evolution of ferroelectric domains under dc electric field and complete 180$^o$ switching in switching-spectroscopy piezoresponse force microscopy. They also exhibit stronger ferromagnetism with nearly an order of magnitude higher saturation magnetization than that of the bulk sample. These results show that the nanoscale BiFeO$_3$ exhibits coexistence of ferroelectric and ferromagnetic order and a strong magnetoelectric multiferroic coupling at room temperature comparable to what some of the type-II multiferroics show at a very low temperature.

cond-mat.str-el↗

arXiv2014

Improper Ferroelectricity in Helicoidal Antiferromagnet Cu3Nb2O8

Cu3Nb2O8 is an unusual multiferroic compound that undergoes a series of magnetic ordering at low temperatures. Concurrent development of electric polarization has been reported at TN1 ~25 K corresponding to a non-collinear helicoidal ordering (Phys. Rev. Lett. 107, 137205 (2011)). But questions remain on the microscopic origin of such phenomena. In this communication, we report a detailed study of induced polar ordering in Cu3Nb2O8 by performing polarization, magnetization, dielectric constant and heat capacity measurements over a broad range of temperature and magnetic field. The dielectric constant shows suppression in the magnetic field but it does not shift to lower temperature with the application of external field. The appearance of magneto-dielectric effect signifies the contribution of q-dependent magnetic correlation function with enhanced weightage in the presence of magnetic field. This magnetic correlation function is associated with the ferro-axial vector and our overall results support this mechanism for the observation of muliferroicity in Cu3Nb2O8.

cond-mat.str-el↗

arXiv2014

Correlation of magneto-electric coupling with crystal structure in Dy doped hexagonal YMnO3

Coexistence of mutually influencing ferroelectric and magnetic ordering at low temperature in hexagonal phase of rare-earth manganites gives rise to interesting physical phenomena. Here, we report a detailed analysis of powder neutron diffraction (ND) studies on polycrystalline Y1-xDyxMnO3 (x = 0, 0.05) as a function of temperature. Our analysis shows that Dy doping at Y site leads to modification in lattice constants: unit cell shrinks in c direction, but expands in ab plane, unit cell volume increases and effective Mn magnetic moment also reduces. All the Mn-O bond lengths and O-Mn-O bond angles shows significant variations leading to reduction in tilting of MnO5 polyhedra. Dielectric measurements on these samples show that, due to Dy doping, inverse S-shape anomaly shifts to the lower temperature side and magnetoelectric coupling decreases. Magnetic measurements confirm the decrease in the frustration of Mn triangular lattice. Temperature dependent specific heat measurement shows anomaly at Néel temperature (TN) and results indicate a decrease in entropy due to Dy doping. These results are understood in terms of modification in magnetoelectric coupling triggered due to Dy induced strain in Y plane of YMnO3.

cond-mat.mtrl-sci↗

arXiv2014

Unconventional magnetism in the spin-orbit driven Mott insulators Ba3MIr2O9 (M=Sc,Y)

We have carried out detailed bulk and local probe studies on the hexagonal oxides Ba3MIr2O9 (M=Sc,Y) where Ir is expected to have a fractional oxidation state of +4.5. In the structure, Ir-Ir dimers are arranged in an edge shared triangular network parallel to the ab plane. Whereas only weak anomalies are evident in the susceptibility data, clearer anomalies are present in the heat capacity data. Our 45Sc nuclear magnetic resonance (NMR) lineshape (first order quadrupole split) is symmetric at room temperature but becomes progressively asymmetric with decreasing temperatures. This is suggestive of distortions in the structure which could arise from progressive tilt/rotation of the IrO6 octahedra with a decrease in temperature T. The 45Sc NMR spectral weight shifts near the reference frequency with decreasing T indicating the development of magnetic singlet regions. Around 10K, a significant change in the spectrum takes place with a large intensity appearing near the reference frequency but with the spectrum remaining multi-peak. It appears from our 45Sc NMR data that in Ba3ScIr2O9 significant disorder is still present below 10K. In the case of Ba3YIr2O9, the 89Y NMR spectral lines are asymmetric at high temperatures but become nearly symmetric (single magnetic environment) below T~70K. Our 89Y spectra and T1 measurements confirm the onset of long range ordering (LRO) from a bulk of the sample at 4K in this compound. Our results suggest that Ba3YIr2O9 might be structurally distorted at room temperature (via, for example, tilt/rotations of the IrO6 octahedra) but becomes progressively a regular triangular lattice with decreasing T. The effective magnetic moments and magnetic entropy changes are strongly reduced in Ba3YIr2O9 as compared to those expected for a S=1/2 system. Similar effects have been found in other iridates which naturally have strong spin-orbit coupling (SOC).

cond-mat.str-el↗

arXiv2013

Neutron diffraction evidence for kinetic arrest of first-order magneto-structural phase transitions in some functional magnetic materials

Neutron diffraction measurements, performed in presence of an external magnetic field, have been used to show structural evidence for the kinetic arrest of the first-order phase transition from (i) the high temperature austenite phase to the low temperature martensite phase in the magnetic shape memory alloy Ni37Co11Mn42.5Sn9.5, (ii) the higher temperature ferromagnetic phase to the lower temperature antiferromagnetic phase in the half-doped charge ordered compound La0.5Ca0.5MnO3 and (iii) the formation of a glass-like arrested state (GLAS). The CHUF (cooling and heating under unequal fields) protocol has been used to establish phase coexistence of metastable and equilibrium states of GLAS and also to demonstrate the devitrification of the arrested metastable states in the neutron diffraction patterns. We also explore the field-temperature (H,T) phase diagram for the two compounds, which depicts the kinetic arrest line TK(H). TK is seen to increase as H increases.

cond-mat.mtrl-sci↗