arXiv subjects

R. J. Choudhary

Publications and source records attributed to R. J. Choudhary.

At least 37 records · Page 2Linked to original sources

arXiv2019

Magneto-dielectric Effect in Relaxor Dipolar Glassy Tb2CoMnO6 Film

We report magneto-dielectric properties of partially B-site ordered monoclinic Tb2CoMnO6 double perovskite thin film epitaxially grown by metalorganic aerosol deposition technique. Transmission electron microscopy and electron energy loss spectroscopy mapping shows the presence and distribution of both Co2+ and Co3+ ions in the film, evidencing a partial B-site disorder, which was further confirmed by the observation of reduced saturation magnetization at low temperatures. The ferromagnetic Curie temperature, TC=110 K, is slightly higher as compared to the bulk value (100 K) probably due to an in plane tensile strain. Remarkably, a short range ordering of spins at T*~190 K>>TC was established and assigned to the B-site disorder in the film. Two different dielectric relaxation peaks have been observed; they merge at the same temperature T* of short range spin correlations. Moreover, an unexpected high temperature dipolar relaxor-glass-like transition at T~T* was observed, at which a coupling to short range magnetic correlations results in a 4% magneto-dielectric coupling.

cond-mat.str-el↗

arXiv2019

Mott-Hubbard insulator-metal transition in the VO2 thin film: A combined XAS and resonant PES study

We have analyzed spectral weight changes in the conduction and the valence band across insulator to metal transition (IMT) in the VO2 thin film using X-ray absorption spectroscopy (XAS) and resonant photoemission spectroscopy (PES). Through temperature dependent XAS and resonant PES measurements we unveil that spectral changes in the d$_{\|}$ states (V 3$\it{d_{x^2-y^2}}$ orbitals) are directly associated with temperature dependent electrical conductivity. Due to presence of the strong electron-electron correlations among the d$_{\|}$ states, across IMT, these states are found to exhibit significant intensity variation compared to insignificant changes in the $π^{\ast}$ and the $σ^{\ast}$ states (which are O 2$\it{p}$ hybridized V 3$\it{d}$ $e_g^π$ and $e_g^σ$ states) in the conduction band. Experimentally obtained values of the correlation parameter (U$_{dd}$ $\sim$ 5.1 eV, intra-atomic V 3$\it{d}$ correlations) and crystal field splitting (10 Dq $\sim$ 2.5 eV) values are used to simulate the V $\it{L_{2,3}}$ edge XAS spectra and an agreement between simulated and experimental spectra also manifests strong correlations. These results unravel that the IMT observed in the VO2 thin film is the Mott-Hubbard insulator-metal transition.

cond-mat.str-el↗

arXiv2019

Hexagonal Sr0.6Ba0.4MnO3: Spin and Dipole Coupling via Local Structure

Hexagonal Sr0.6Ba0.4MnO3 (SBMO) follows P63/mmc symmetry where MnO6 octahedra are both face-shared (Mn2O9 bi-octahedra) and corner-shared via oxygen anion. It undergoes ferroelectric (FE) and antiferromagnetic (AFM) orderings close to the room temperature. Magnetic properties appear to be governed by intricate exchange interactions among Mn4+ ions within and in adjacent Mn2O9 bi-octahedra, contingent upon the local structural changes. Calculations based on our model spin-Hamiltonian reveal that the dominant linear AFM fluctuations between the Mn4+ ions of two oxygen-linked bi-octahedra result in short range correlations, manifest as a smooth drop in magnetization below 325 K. Competition between spin-exchange and local-strain is reckoned as responsible for the atypical magneto-electricity, obtained near the room temperature.

cond-mat.mtrl-sci↗

arXiv2019

Tuning the Magnetic Ground State by Charge Transfer Energy in SrCoO2.5 via Strain Engineering

SrCoO2.5 (SCO) is a charge transfer insulator with 3d6 ground state configuration leading to antiferromagnetic nature. It is observed that substrate induced strain engineering modifies the ground state of SCO thin film with 3d7L (L:O-2p hole) configuration causing negative charge transfer energy.The consequent strong hybridization between O-2p and Co-3d bands causes a hole in O-2p band leading to hole mediated unconventional ferromagnetic ordering in SrCoO2.5 thin film. This opens up a new avenue to tune the electronic structure vis a vis magnetic property via strain engineering.

cond-mat.str-el↗

arXiv2019

Phonon Invisibility Driven by Robust Magneto-Elastic Coupling in AlFeO3 Thin Film

The thin films of lead free magneto-electric compound AlFeO3 have been deposited using pulsed laser deposition technique. X-ray diffraction, X-ray absorption spectroscopy and reflectivity measurements established the orthorhombic structure and material density of 4.5g/cc which is comparable with bulk AlFeO3. The Raman mode corresponding to AlFeO3 was found to vanish when magnetic field of 800 Oe was applied at room temperature. Additionally, it was observed that the Raman phonon mode present at the room temperature becomes invisible in the temperature window of 280K-236K and reappears below it. The detailed analysis of magnetization showed a change in magnetic order in this temperature interval. The invisibility of Raman phonon mode corresponding to AlFeO3 have been attributed to the lattice deformation caused by the magnetoelastic effect. The presence of strong spin-lattice coupling is also validated by the renormalization of phonon frequencies below 200 K.

cond-mat.mtrl-sci↗

arXiv2019

Role of local short-scale correlations in the mechanism of negative magnetization

We elaborate here why the antiferromagnetically ordered GdCrO$_3$ responds in a diamagnetic way under certain conditions, by monitoring the evolution of the microscopic global and local magnetic phases. Using high energy $\sim$ 0.3 eV neutrons, the magnetic ordering is shown to adopt three distinct magnetic phases at different temperatures: G$_x^{Cr}$,A$_y^{Cr}$,F$_z^{Cr}$ below Néel temperature = 171 K; (F$_x^{Cr}$, C$_y^{Cr}$, G$_z^{Cr}$)$\bullet$( F$_x$$^{Gd}$,C$_y$$^{Gd}$) below 7 K and an intermediate phase for 7 K $ \le T \le$ 20 K in the vicinity of spin-reorientation phase transition. Although, bulk magnetometry reveals a huge negative magnetization (NM) in the terms of both magnitude and temperature range ( $M_{- max}$ ( 18 K)$\sim$ 35 $\times M_{+ max}$ (161 K), $ΔT \sim 110$ K in presence of $μ_0H$ = 0.01 T); the long-range magnetic structure and derived ordered moments are unable to explain the NM. Real-space analysis of the total (Bragg's + diffuse) scattering reveals significant magnetic correlations extending up to $\sim$ 9 $Å$. Accounting for these short-range correlations with a spin model reveals spin frustration in the S= 3 ground state, comprising competing first, second and third next nearest exchange interactions with values J$_1$ = 2.3 K, J$_2$ = -1.66 K and J$_3$ = 2.19 K in presence of internal field, governs the observance of NM in GdCrO$_{3}$.

cond-mat.mtrl-sci↗

arXiv2018

Interfacial spin glass mediated unusual spontaneous exchange bias effect in epitaxial self-assembled La0.7Sr0.3MnO3:NiO nanocomposite thin films

Zero field cooled spontaneous exchange bias (SEB) is observed in epitaxial La0.7Sr0.3MnO3 (LSMO):NiO self-assembled nanocomposite thin films grown on (001) SrTiO3 single crystal substrate by pulsed laser deposition. SEB is displayed by the novel asymmetry in the hysteresis loop of the composite film along with the field cooled conventional exchange bias (CEB) effect. The training effect shows that exchange bias relaxation is disorder mediated. It is revealed from DC magnetization results that such nanocomposite film divulges spin glass like behaviour, which is arising due to competing ferromagnetic and antiferromagnetic inteactions at the assorted interfaces of ferromagnetic LSMO and antiferromagnetic NiO. Also corroborated by x-ray magnetic circular dichroism (XMCD) measurements, we conclude that SEB is mainly originating due to ferromagnetic coupling of unstable interfacial antiferromagnetic spin due to NiO with the ferromagnetic LSMO at the disordered interface. These results of self-assembled thin films provide a useful input to realize and understand microscopic origin of SEB for device application.

cond-mat.mtrl-sci↗

arXiv2018

Spin-lattice coupling mediated giant magnetodielectricity across the spin reorientation in Ca2FeCoO5

The structural, phonon, magnetic, dielectric, and magneto dielectric responses of the pure bulk Brownmillerite compound Ca2FeCoO5 are reported. This compound showed giant magneto dielectric response (10%-24%) induced by strong spin-lattice coupling across its spin reorientation transition (150-250 K). The role of two Debye temperatures pertaining to differently coordinated sites in the dielectric relaxations is established. The positive giant magneto-dielectricity is shown to be a direct consequence of the modulations in the lattice degrees of freedom through applied external field across the spin reorientation transition. Our study illustrates novel control of magneto-dielectricity by tuning the spin reorientation transition in a material that possess strong spin lattice coupling.

cond-mat.mtrl-sci↗

arXiv2018

Effect of magnetic and non-magnetic impurities on the spin dimers in the spin 1/2 chains of quantum magnet Sr$_{14}$Cu$_{24}$O$_{41}$

We study the effect of impurities on the two types of spin-dimers in the hybrid chain/ladder spin 1/2 quantum magnet Sr$_{14}$Cu$_{24}$O$_{41}$. Four different impurities were used, namely, the non-magnetic Zn (0.0025 and 0.01 per Cu) and Al (0.0025 and 0.01 per Cu), and magnetic Ni (0.0025 and 0.01 per Cu) and Co (0.01, 0.03, 0.05 and 0.1 per Cu). These impurities were doped in high-quality single-crystals synthesized by the floating zone method. The magnetic susceptibility of pristine Sr$_{14}$Cu$_{24}$O$_{41}$ is analyzed rigorously to confirm that at low temperatures (T $<$ 5 K), the "free" spins in the chains undergo a long-distance dimerization as proposed in a recent study [Sahling et al. Nature Phys., \textbf{11}, 255 (2015)]. The effect of impurity on these dimers is analyzed by measuring the specific heat down to T = 0.06 K. We found that even at the lower impurity concentration, the long-distance dimers are significantly severed, but the quantum entangled spin dimerized state of the chains persists. On the other hand, the other type of spin dimers that forms at relatively higher temperatures via an intervening Zhang-Rice singlet are found to be practically unaffected at the lower impurity concentration; but at 1\% doping, even these are found to be considerably severed. The effect of Co impurity turned out to be most unusual displaying a strongly anisotropic response, and with a dimerization gap that suppresses faster along the chain/ladder direction than perpendicular to it as a function of increasing Co concentration.

cond-mat.str-el↗

arXiv2018

Nature of magnetism and transport in BxCyNz thin films: The intriguing role of nitrogen defects in the electronic structure

Boron carbonitride (BxCyNz) represents an interesting family of materials containing all light elements and two dimensional graphene like hybrid layers. Although rich literature exists on this peculiar material in chemically processed form, there are relatively fewer reports on device application-worthy thin film form. This form also offers a natural platform for basic studies on important aspects such as magnetism and transport, which have attracted attention in the context of ferromagnetism in doped and defect carbon systems. Thus, in this work we have grown thin films of this compound using Pulsed Laser Deposition (PLD) method, and investigated their magnetic and transport properties in their entirety along with the detailed electronic structure using various spectroscopic techniques like X-ray photoelectron spectroscopy (XPS), Valence Band Spectroscopy (VBS) and X-ray absorption near edge spectroscopy (XANES). In depth analysis of the typical role of dopants and defects, especially the prevalent nitrogen defects, is elucidated using Density Functional Theory (DFT) calculations to understand the experimental observations. A dramatic crossover in the transport mechanism of charge carriers is observed in this system with the change in doping level of specific nitrogen defects. A robust and high saturation magnetization is achieved in BCN films which is higher by almost hundred times as compared to that in similarly grown undoped carbon film. An anomalous transition and increase in coercive field is also observed at low temperature. A careful analysis brings out the intriguing role of specific nitrogen defects in defining the peculiar nature and concentration dependence of the physical properties of this system.

cond-mat.mtrl-sci↗

arXiv2018

Multiferroicity and magnetoelastic coupling in alpha-Mn2O3: A binary perovskite

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 alpha-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 alpha-Mn2O3 provides insights for the exploration of ME coupling in related materials.

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↗

arXiv2017

Sign reversal of magnetoresistance and p to n transition in Ni doped ZnO thin film

We report the magnetoresistance and nonlinear Hall effect studies over a wide temperature range in pulsed laser deposited Ni0.07Zn0.93O thin film. Negative and positive contributions to magnetoresistance at high and low temperatures have been successfully modeled by the localized magnetic moment and two band conduction process involving heavy and light hole subbands, respectively. Nonlinearity in the Hall resistance also agrees well with the two channel conduction model. A negative Hall voltage has been found for T $\gte 50 K$, implying a dominant conduction mainly by electrons whereas positive Hall voltage for T less than 50 K shows hole dominated conduction in this material. Crossover in the sign of magnetoresistance from negative to positive reveals the spin polarization of the charge carriers and hence the applicability of Ni doped ZnO thin film for spintronic applications.

cond-mat.mtrl-sci↗

arXiv2015

Evidence of ferromagnetic short-range correlations in cubic La1-xSrxMnO3-δ (x=0.80, 0.85) above antiferromagnetic ordering

We report the existence of ferromagnetic correlations (FMC) in paramagnetic (PM) matrix of cubic La1-xSrxMnO3-δ (x = 0.80, 0.85) well above its coupled structural, magnetic and electronic phase transitions. The dc-magnetization vs temperature [M(T)] behaviour under different magnetic fields (from 100 Oe to 70 kOe) shows the presence of short range magnetic correlations up to (TFMC ~) 365 K, far above the antiferromagnetic ordering temperatures (TN =) 260 K and 238 K for x=0.80 and 0.85, respectively. More importantly the observed short-range FMC survive even up to 70 kOe, which indicates their robust nature. The temperature region between TN to TFMC is dominated by the presence of correlated ferromagnetic (FM) entities within the PM matrix and stabilized due to A-site chemical disorder. Our results further illustrate that for the studied compositions, the oxygen off-stoichiometry does not have any significant effect on the nature and strength of these FM entities; however, FM interactions increase in the oxygen deficient samples. These compositions are the unique examples, where the presence of FMC is observed in an undistorted basic cubic perovskite lattice well above TN and therefore are novel to understand the physics behind the colossal magneto-resistance effect.

cond-mat.str-el↗

arXiv2014

Oxygen deficiency induced suppression of JT-distortion and stabilization of chargeordering in La0.2Sr0.8MnO3-d

Structural phase transition studies employing low-temperature transmission electron microscopy, and low-temperature x-ray diffraction have been carried out on nearly stoichiometric (δ=0.01) and off-stoichiometric (δ=0.12) versions of La0.2Sr0.8MnO3-δ manganite. The nearly stoichiometric La0.2Sr0.8MnO3-δ under goes a cubic to Jahn-Teller distorted C-type antiferromagnetic tetragonal phase-transition at 260K. For off-stoichiometric La0.2Sr0.8MnO3-δ the Jahn-Teller distorted tetragonal phase transition gets totally suppressed and the basic perovskite lattice remains cubic but shows a charge ordered phase. Stabilization of charge ordered phase in the absence of cooperative Jahn-Teller distortion has been attributed to coulomb-repulsion and Hunds coupling energy. The off-stoichiometric sample shows characteristically different physical properties. This has been realized through transport, magnetic and calorimetric measurements. A smooth crossover from variable range hopping transport to power-law dependence of resistivity (ρ) on temperature (T) i.e. ρ=C.T-α has been realized. This has been attributed to multistep inelastic tunneling through channels involving localized states around oxygen vacancy sites.

cond-mat.str-el↗

arXiv2013

Modification in structural, dielectric and magnetic properties of La and Nd co-substituted epitaxial BiFeO3 thin films

The influence of La and Nd co-substitution on the structural and magnetic properties of BiFeO3 (BFO) thin films was examined. Epitaxial thin films of pure and, La and Nd co-doped BFO on the SrRuO3 buffered single crystal SrTiO3 (001) substrate were deposited using pulsed laser deposition. The structural change in co doped La and Nd BFO thin films which was caused by the changes of force constant in the crystal lattice induced by ionic radii mismatch was investigated. Raman spectroscopy studies manifest the structural change in doped BFO films from rhombohedral to monoclinic distorted phase which is induced by the co substitution of La and Nd. Room temperature magnetic hysteresis curves indicated that saturation magnetization is enhanced in the doped film with saturation magnetization of ~20 emu/cm3. The dielectric and magnetic properties are effectively improved in BLNFO films compared to pure BFO thin films.

cond-mat.mtrl-sci↗

arXiv2013

Crossover from injection to tunneling conduction mode and associated magneto-resistance in a single $Fe_{3}O_{4}$(111)/$Alq_{3}$/Co spin-valve device

We demonstrate interface energy level engineering, exploiting the modification in energy band structure across Verwey phase transition of $Fe_{3}O_{4}$ electrode, in a $Fe_{3}O_{4}$(111)/$Alq_{3}$/Co vertical spin-valve (SV) device. Experimental results on device characteristics I-V) study exhibit a transition in conduction mode from carrier injection to tunneling across Verwey transition temperature ($T_{V}$) of $Fe_{3}O_{4}$ electrode. Both giant magneto-resistance (GMR) and tunneling MR (TMR) have been observed in a single SV device as a function of temperature, below and above $T_{V}$, respectively. Appearance of GMR, accompanied by injection limited natural Schottky-like I-V characteristics, provide evidences of spin injection at electrode/$Alq_{3}$ interface and transport through molecular orbitals in this SV device. Features of TMR exhibit significant differences from that of GMR. This is due to the dominant hyperfine-field interaction in the multi-step tunneling regime. We have achieved room-temperature SV operation in our device. A phenomenological model for device operation has been proposed to explain the transition in the conduction mode and associated MR features across $T_{V}$. We propose that the tuning of charge gap at Fermi level across Verwey transition due to charge ordering on the octahedral iron sites of $Fe_{3}O_{4}$ results in a corresponding tuning of conduction mode causing this unique cross over from GMR to TMR in this ferrite-based organic SV.

cond-mat.mes-hall↗

arXiv2011

Effect of non-magnetic impurities on the magnetic states of anatase TiO$_2$

The electronic and magnetic properties of TiO$_2$, TiO$_{1.75}$, TiO$_{1.75}$N$_{0.25}$, and TiO$_{1.75}$F$_{0.25}$ compounds have been studied by using \emph{ab initio} electronic structure calculations. TiO$_2$ is found to evolve from a wide-band-gap semiconductor to a narrow-band-gap semiconductor to a half-metallic state and finally to a metallic state with oxygen vacancy, N-doping and F-doping, respectively. Present work clearly shows the robust magnetic ground state for N- and F-doped TiO$_2$. The N-doping gives rise to magnetic moment of $\sim$0.4 $μ_B$ at N-site and $\sim$0.1 $μ_B$ each at two neighboring O-sites, whereas F-doping creates a magnetic moment of $\sim$0.3 $μ_B$ at the nearest Ti atom. Here we also discuss the possible cause of the observed magnetic states in terms of the spatial electronic charge distribution of Ti, N and F atoms responsible for bond formation.

cond-mat.str-el↗