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R. J. Choudhary

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

At least 19 recordsLinked to original sources

Room temperature reversible colossal volto-magnetic effect in all-oxide metallicmagnet/topotactic-phase-transition material heterostructures

Multiferroic materials have undergone extensive research in the past two decades in an effort to produce a sizable room-temperature magneto-electric (ME) effect in either exclusive or composite materials for use in a variety of electronic or spintronic devices. These studies have looked into the ME effect by switching the electric polarization by the magnetic field or switching the magnetism by the electric field. Here, an innovative way is developed to knot the functional properties based on the tremendous modulation of electronics and magnetization by the electric field of the topotactic phase transitions (TPT) in heterostructures composed of metallic-magnet/TPT-material. It is divulged that application of a nominal potential difference of 2-3 Volts induces gigantic changes in magnetization by 100-250% leading to colossal Voltomagnetic effect, which would be tremendously beneficial for low-power consumption applications in spintronics. Switching electronics and magnetism by inducing TPT through applying an electric field requires much less energy, making such TPT-based systems promising for energy-efficient memory and logic applications as well as opening a plethora of tremendous opportunities for applications in different domains.

cond-mat.mtrl-sci↗

Random magnetic anisotropy driven transitions in layered perovskite LaSrCoO$_4$

Attempts to unravel the nature of magnetic ordering in LaSrCoO$_4$ (Co$^{3+}$), a compound intermediate between antiferromagnetic (AFM) La$_2$CoO$_4$ (Co$^{2+}$) and ferromagnetic (FM) Sr$_2$CoO$_4$ (Co$^{4+}$), have met with a limited success so far. In this report, the results of a thorough investigation of dc magnetization and ac susceptibility (ACS) in single-phase LaSrCoO$_4$ provide clinching evidence for a thermodynamic paramagnetic (PM) - ferromagnetic (FM) phase transition at T$_{c}$ = 220.5 K, followed at lower temperature (T$_{g}$ = 7.7 K) by a transition to the cluster spin glass (CSG) state. Analysis of the low-field Arrott plot isotherms, in the critical region near T$_{c}$, in terms of the Aharony-Pytte scaling equation of state clearly establishes that the PM-FM transition is basically driven by random magnetic anisotropy (RMA). For temperatures below $\approx$ 30 K, large enough RMA destroys long-range FM order by breaking up the infinite FM network into FM clusters of finite size and leads to the formation of a CSG state at temperatures T $\lesssim$ 8 K by promoting freezing of finite FM clusters in random orientations. Increasing strength of the single-ion magnetocrystalline anisotropy (and hence RMA) with decreasing temperature is taken to reflect an increase in the number of low-spin (LS) Co$^{3+}$ ions at the expense of that of high-spin (HS) Co$^{3+}$ ions. At intermediate temperatures (30 K $\lesssim T \lesssim$ 180 K), spin dynamics has contributions from the infinite FM network (fast relaxation governed by a single anisotropy energy barrier) and finite FM clusters (extremely slow stretched exponential relaxation due to hierarchical energy barriers).

cond-mat.mtrl-sci↗

Temperature and terahertz frequency dependence of the dielectric properties of Fe3O4 thin films deposited on Si substrate

The Fe$_3$O$_4$/Si films are considered to be promising materials for THz spintronic applications due to their high temperature magnetic transition and semiconducting properties. In this article, we present the real part of the dielectric constant ($ε_1$) and the optical conductivity ($σ_1$) of Fe$_3$O$_4$ films of different thicknesses deposited on Si substrate (Fe$_3$O$_4$/Si) in the THz range at temperatures 2- 300 K. Although the magnetization of the films with thickness $\geq$ 115 nm shows a clear change at the Verwey transition temperature T$_v$ = 121 K, their optical properties in the THz frequency range are drastically different from each other. We have shown that $σ_1$ is maximum and $ε_1$ is minimum when the Fe$^{+2}$/Fe$^{+3}$ ratio is equal to 0.54 which is the ratio of Fe+2/Fe+3 for pure Fe$_3$O$_4$. The $σ_1$ reduces and $ε_1$ increases at all temperatures when the Fe$^{+2}$/Fe$^{+3}$ ratio deviates from 0.54. We have shown that a slight change in the Fe$^{+2}$/Fe$^{+3}$ ratio can induce large changes in the optical properties which shall have implications in the application of the Fe3O4 films in THz spintronics.

cond-mat.mtrl-sci↗

Photosensitive SrMnO3

In recent years, photosensitive materials have been in huge demand because of their fascinating ability to convert absorbed photon energy to generate strain and henceforth tuning the physical properties. In this report we detect the photosensitive activity of SrMnO3. Using the power dependent and temperature dependent Raman study with different laser sources having wavelengths across the optical band gap of SrMnO3, we divulge the photosensitive character of SrMnO3 thin films. Upon laser light illumination, Raman modes soften and softening further increases with increase in laser power. Similar kind of mode variation is observed with increasing temperature at fixed laser power. XAS in presence of laser illumination, reveals the change in crystal field splitting associated with mode softening.

cond-mat.mtrl-sci↗

Exchange bias in Sm$ _{2} $NiMnO$ _{6}$/BaTiO$ _{3}$ ferromagnetic-diamagnetic heterostructure thin films

Exchange bias (EB) shifts are commonly reported for the ferromagnetic (FM)/antiferromagnetic (AFM) bilayer systems. While stoichiometric ordered Sm$_{2}$NiMnO$_{6}$ (SNMO) and BaTiO$_{3}$ (BTO) are known to possesses FM and diamagnetic orderings respectively, here we have demonstrated the cooling field dependent EB and training effects in epitaxial SNMO/BTO/SNMO (SBS) heterostructure thin films. The polarized Raman spectroscopy and magnetometric studies reveal the presence of anti-site cation disorders in background of ordered lattice in SNMO layers, which introduces Ni-O-Ni or Mn-O-Mn local AFM interactions in long range Ni-O-Mn FM ordered host matrix. We have also presented growth direction manipulation of the degree of cation disorders in the SNMO system. Polarization dependent X-ray absorption measurements, duly combined with configuration interaction simulations suggest charge transfer from Ni/Mn 3\textit{d} to Ti 3\textit{d} orbitals through O 2\textit{p} orbitals across the SNMO/BTO (SB) interfaces, which can induce magnetism in the BTO spacer layer. The observed exchange bias in SBS heterostructures is discussed considering the pinning of moments due to exchange coupling at SB (or BTO/SNMO) sandwich interface.

cond-mat.mtrl-sci↗

Magnetic properties of disordered polycrystalline bulk Sm$ _{2} $NiMnO$ _{6} $ double perovskite

The structural, electronic and magnetic properties of anti-site disordered Sm$ _{2} $NiMnO$ _{6} $ double perovskite has been studied. RE$_{2}$NiMnO$_{6}$ (RE: rare-earth) ordered double perovskite is commonly believed to show two distinct magnetic phase transitions viz, paramagnetic to ferromagnetic (FM) transition at T = T$ _{C} $ due to Ni-O-Mn super exchange interaction and another transition at T = T$ _{d} $ due to coupling of RE spins with Ni-Mn network. In our present study, we have observed that the presence of intrinsic B-site disorder results in an additional antiferromagnetic (AFM) coupling, mediated via Ni-O-Ni and Mn-O-Mn local bond pairs. As a consequence, the magnetic behavior of SNMO comprises of co-existing FM-AFM phases, which are respectively governed by the anti-site ordered and disordered structures. Field dependent inverted cusp like trend in M(T) and two step reversible loop behavior in M(H) measurements indicate the presence of competing FM-AFM phases over a wide range of temperature values (T$ _{d} < $ T $ < $ T$ _{C} $).

cond-mat.mtrl-sci↗

Existence of inter coupled structural, electronic and magnetic states in Sm$ _{2} $NiMnO$ _{6} $ double perovskite

Coupling between different interactions allows to control physical aspects in multifunctional materials by perturbing any of the degrees of freedom. Here, we aim to probe the correlation among structural, electronic and magnetic observables of Sm$ _{2} $NiMnO$ _{6} $ ferromagnetic insulator double perovskite. Our employed methodology includes thermal evolution of synchrotron X-ray diffraction, near edge and extended edge hard X-ray absorption spectroscopy and bulk magnetometry. The magnetic ordering in SNMO adopts two transitions, at T$ _{C} $=159.6K due to ferromagnetic arrangement of Ni-Mn sublattice and at T$ _{d} $=34.1K because of anti-parallel alignment of polarized Sm paramagnetic moments with respect to Ni-Mn network. The global as well as local crystal structure of SNMO undergoes isostructural transitions across T$ _{C} $ and T$ _{d} $, observed by means of temperature dependent variation in Ni/Mn-O, Ni-Mn bonding characters and super exchange angle in Ni-O-Mn linkage. Hybridization between Ni, Mn 3\textit{d}, O 2\textit{p} electronic states is also modified in the vicinity of magnetic transition. On the other hand, the signature of Ni/Mn anti-site disorders are evidenced from local structure and magnetization analysis. The change in crystal environments governs the magnetic response by imposing alteration in metal - ligand orbital overlap. Utilizing these complimentary probes we have found that structural, electronic and magnetic states are inter-coupled in SNMO which makes it a potential platform for technological usage.

cond-mat.mtrl-sci↗

Probing the electronic and local structure of Sr$_{2-x}$La$_x$CoNbO$_6$ using near-edge and extended x-ray absorption fine structures

We report the electronic and local structural investigation of double pervoskites Sr$_{2-x}$La$_x$CoNbO$_6$ ($x=$ 0--1) using x-ray absorption near edge structure (XANES) and extended x-ray absorption fine structures (EXAFS) at the Nb, Co, and Sr $K$-edges. The $ab$ $initio$ simulations and detailed analysis of the Nb and Co $K$-edge XANES spectra demonstrate that the observed pre-edge features arise from the transition of 1$s$ electrons to the mixed $p-d$ hybridized states. We reveal a $z$-out Jahn-Teller (JT) distortion in the CoO$_6$ octahedra, which decreases monotonically due to an enhancement in the JT inactive Co$^{2+}$ ions with $x$ . On the other hand, the $z$-in distortion in NbO$_6$ octahedra remains unaltered up to $x=$ 0.4 and then decreases with further increase in $x$. This sudden change in the local coordination around Nb atoms is found to be responsible for the evolution of the antiferromagnetic interactions in $x \geqslant$ 0.6 samples. Also, we establish a correlation between the degree of octahedral distortion and intensity of the white line feature in the XANES spectra and possible reason for this are discussed. More interestingly, we observe the signature of KN$_1$ double electron excitation in the Sr $K$-edge EXAFS spectra for all the samples, which is found to be in good agreement with the $Z$+1 approximation. Further, the Co L$_{2,3}$ edge shows the reduction in the crystal field strength and hence an increase in the charge transfer energy ($Δ_{ct}$) with the La substitution.

cond-mat.str-el↗

Microscopic insights of magnetism in Sm$ _{2} $NiMnO$ _{6} $ double perovskite

The functional characteristics of double perovskites with unique ferromagnetic-insulator ground state have been controversial due to the unavoidable presence of anti-site disorders (ASDs). Here, we aim to investigate the origin of magnetic ordering on local and global scales in Sm$_{2}$NiMnO$_{6}$ (SNMO) double perovskite system. Different calcination routes are exploited to generate different cation arrangements in SNMO and the corresponding magnetic configurations are examined using the high energy (E $ \sim $0.3 eV) `hot neutrons', which has helped to overcome Sm absorption as well as to record total (Bragg's+diffuse) scattering profiles with high momentum transfer (Q$ _{max} \sim $24 angstrom$ ^{-1} $). We have observed that the Ni-Mn sublattice adopts long range collinear ferromagnetic $ F_{x}F_{z} $ structure with commensurate $k$=(0, 0, 0) propagation vector, below ordering temperature T $ \lesssim $ 160 K, irrespective of variable ASD concentrations. In addition, the signatures indicating the antiparallel polarization of Sm paramagnetic moments with respect to Ni-Mn network, are noticed in the vicinity of anomalous magnetic transitions at T $ \lesssim $ 35 K. The real space pair distribution function calculations have provided a direct visualization of ASDs by means of broadening in Ni/Mn-Mn/Ni linkage. Employing the Reverse Monte Carlo approach on diffuse magnetic scattering profiles, we have observed the negative spin-spin correlation function which suggests the Ni-Ni antiferromagnetic exchange interactions ranging up to first nearest neighbor distance. These results confirm that the existence of ASDs in cation ordered host matrix leads to competing ferromagnetic-antiferromagnetic phases in a broad temperature range, which quantitatively governs the temperature dependent bulk magnetic observables of SNMO system.

cond-mat.mtrl-sci↗

Correlation between spin-phonon coupling and magneto-electric effects in CoFe2O4/PMN-PT nanocomposite: Raman Spectroscopy and XMCD study

We have investigated the coupling of lattice with spin via strain interactions in the CoFe2O4/PMN-PT composite system. X-ray diffraction and Raman spectroscopic studies illustrate a remarkable modification in CoFe2O4lattice across Curie temperature (450 K) of PMN-PT. Subsequently, CoFe2O4/PMN-PT composite reveals a sudden drop in magnetic moment across Tc of PMN-PT (450 K). However,theindependent CoFe2O4phasedisplaystypical ferromagnetic behaviour across this temperature. These findings establish spin-lattice coupling owing to th interfacial strain transfer between CoFe2O4 and PMN-PT in composite. The strain intractions leads to magneto-electric coupling, evidenced by measuring magentization and magneto-electric coefficient for the electric field poled and unploed CoFe2O4/PMN-PT composite samples. X-ray magnetic circular dichroism (XMCD) analysis establishes that the cation (Fe3+/Co2+) redistribution occurs on tetrahedral and octahedral site in the electrically poled CoFe2O4/PMN-PT composite, confirming the coupling between magnetic and electric ordering in the composite. The magneto-electric coupling coefficient alpha vs dc magnetic field curves revealed hysteretic behavior and enhanced α values after electric poling, which originates from the strain induced modifications in the magnetic domains configuration of composite in the poled samples. These findings suggest that the existence of spin lattice coupling may leads to the mechanism of strong magneto-electric effects via strain interactions in CoFe2O4/PMN-PT composite.

cond-mat.mtrl-sci↗

Strain assisted magnetization switching in ordered nanomagnets of CoFe2O4/SrRuO3/PMNPT hetrostructures

We have explored the electric field controlled magnetization in the nanodot CoFe2O4/SrRuO3/PMN-PT heterostructures. Ordered ferromagnetic CFO nanodots (~300 nm lateral dimension) are developed on the PMN-PT substrate (ferroelectric as well as piezoelectric) using a nanostencil-mask pattering method during pulsed laser deposition. The nanostructures reveal electric field induced magnetization reversal in the single domain CFO nanodots through transfer of piezostrains from the piezoelectric PMN-PT substrate to the CFO. Further, electric field modulated spin structure of CFO nanomagnets is analysed by using X-ray magnetic circular dichroism (XMCD). The XMCD analysis reveals cations (Fe3+/Co2+) redistribution on the octahedral and tetrahedral site in the electric field poled CoFe2O4 nanodots, establishing the strain induced magneto-electric coupling effects. The CoFe2O4/SrRuO3/PMN-PT nanodots structure demonstrate multilevel switching of ME coupling coefficient (α) by applying selective positive and negative electric fields in a non-volatile manner. The retention of two stable states of α is illustrated for ~106 seconds, which can be employed to store the digital data in non-volatile memory devices. Thus the voltage controlled magnetization in the nanodot structures leads a path towards the invention of energy efficient high-density memory devices.

cond-mat.mtrl-sci↗

Mapping the magnetic state as a function of anti-site disorder in Sm$ _{2} $NiMnO$ _{6} $ double perovskite thin films

The predictability of any characteristic functional aspect in a double perovskite system has always been compromised by its strong dependence over the inevitably present anti-site disorders (ASD). Here, we aim to precisely map the quantitative and qualitative nature of ASD with the corresponding modifications in observables describing the magnetic and electronic state in epitaxial Sm$ _{2} $NiMnO$ _{6} $ (SNMO) double perovskite thin films. The concentration and distribution patterns of ASD are effectively controlled by optimizing growth conditions and estimated on both local and global scales utilizing extended X-ray absorption fine structure and bulk magnetometry. Depending upon the defect densities, the nature of disorder distribution can vary from homogeneous to partially segregated patches. Primarily, the effect of varying B-site cationic arrangement in SNMO is reflected as the competition of long range ferromagnetic (FM) and short scale antiferromagnetic (AFM) interactions originated from ordered Ni-O-Mn and disordered Ni-O-Ni or Mn-O-Mn bonds, respectively, which leads to systematic shift in magnetic transition temperature and drastic drop in saturation magnetization. In addition, we have observed that the gradual increment in density of ASD leads to significant deviation from uniaxial anisotropy character, reduction in anisotropy energy and enhancement of moment pinning efficiency. However, the observed signatures of $ Ni^{2+}+Mn^{4+} \longrightarrow Ni^{3+}+Mn^{3+} $ charge disproportionation is found to be independent of cation disorder densities. This work serves as a basic route-map to tune the characteristic magnetic anisotropy, magnetic phase transitions, and magnetization reversal mechanism by controlling ASD in a general double perovskite system.

cond-mat.mtrl-sci↗

Robust perpendicular magnetic anisotropy in Ce substituted yttrium iron garnet epitaxial thin films

Cerium substituted yttrium iron garnet (Ce:YIG) epitaxial thin films are prepared on gadolinium gallium garnet (GGG) substrate with pulsed laser deposition (PLD). It is observed that the films grown on GGG(111) substrate exhibit perpendicular magnetic anisotropy (PMA) as compared to films grown on GGG(100) substrate. The developed PMA is confirmed from magneto-optical Kerr effect, bulk magnetization and ferromagnetic resonance measurements. Further, the magnetic bubble domains are observed in the films exhibiting PMA. The observations are explained in terms of the growth direction of Ce:YIG films and the interplay of various magnetic anisotropy terms. The observed PMA is found to be tunable with thickness of the film and a remarkable temperature stability of the PMA is observed in all the studied films of Ce:YIG deposited on GGG(111) substrate.

cond-mat.mtrl-sci↗

Role of electronic excitation on the anomalous magnetism of elemental Copper

Magnetic susceptibility of elemental copper (Cu) shows an anomalous rise at low temperatures superimposed on the expected atypical diamagnetic response. Such temperature dependent susceptibility, which is also known as the Curie tail, can not be explained on the basis of Larmor diamagnetic and Pauli paramagnetic contributions expected in Cu. Using valence band resonant photoemission spectroscopy results and density functional theory calculations, we show the magnetic anomaly appears due to presence of holes in Cu 3d band, which originates from thermally excited electronic configuration. Our study therefore highlights that the Curie tail, which is generally overlooked presuming it either due to paramagnetic impurities or defects, can in fact be intrinsic to a material, and even simple systems like elemental Cu is susceptible to electronic excitations giving rise to anomalous magnetic state.

cond-mat.mtrl-sci↗

Spectroscopic comprehension of Mott-Hubbard insulator to negative charge transfer metal transition in LaNi_{x}V_{1-x}O_{3} thin films

The room temperature (300 K) electronic structure of pulsed laser deposited LaNi_{x}V_{1-x}O_{3} thin films have been demonstrated. The substitution of early-transition metal (TM) V in LaVO_{3} thin films with late-TM Ni leads to the decreasing in out-of-plane lattice parameter. Doping of Ni does not alter the formal valence state of Ni and V in LaNi_{x}V_{1-x}O_{3} thin films, divulging the absence of carrier doping into the system. The valence band spectrum is observed to comprise of incoherent structure owing to the localized V 3d band along with the coherent structure at Fermi level. With increase in Ni concentration, the weight of the coherent feature increases, which divulges its origin to the Ni 3d-O 2p hybridized band. The shift of Ni 3d-O 2p hybridized band towards higher energy in Ni doped LaVO_{3} films compared to the LaNiO_{3} film endorses the modification in ligand to metal charge transfer (CT) energy. The Ni doping in Mott-Hubbard insulator LaVO_{3} leads to the closure of Mott-Hubbard gap by building of spectral weight that provides the delocalized electrons for conduction. A transition from bandwidth control Mott-Hubbard insulator LaVO_{3} to negative CT metallicity character in LaNiO_{3} film is observed. The study reveals that unlike in Mott-Hubbard insulators where the strong Coulomb interaction between the 3d electrons decides the electronic structure of the system, CT energy can deliver an additional degree of freedom to optimize material properties in Ni doped LaVO_{3} films.

cond-mat.str-el↗

Enhanced charge-transfer character in the monoclinic phase of Mott-insulator LaVO3 thin film

Electronic structure of pulsed laser deposited epitaxial LaVO3 (LVO) thin film grown on LaAlO3 (001) (LAO) substrate, has been studied at room temperature and at 130 K, which is below the structural (141 K) and magnetic transition temperatures (143 K) of single crystal LVO. Significant modification in spectral intensity, largely around the V 3d - O 2p hybridized region, is observed in valence band spectrum (VBS) of LVO film at 130 K. Resonant photoemission study at 130 K confirms the presence of charge transfer screened 3dnL (L: hole in the O 2p) final state along with the dominant 3dn-1 final state at 1.5 eV binding energy in the valence band. On the contrary, in the room temperature VBS dominant V 3d sates with only 3dn-1 kind final state is accentuated. To understand this difference, density functional theory (DFT) calculations are employed. The changes in crystal structure from room temperature orthorhombic (O-LVO) to low temperature monoclinic (M-LVO) symmetry leads to remarkable change in the electronic structure around the Fermi level, including transition from direct to indirect nature of band gap. Our calculations also confirm an enhanced O 2p character in the valence band edge of M-LVO that is hybridized with V 3d. These results are further corroborated with octahedral distortions associated with the structural transition.

cond-mat.str-el↗

Role of Ni substitution on structural, magnetic and electronic properties of epitaxial CoCr2O4 spinel thin films

Cubic spinel CoCr2O4 has attained recent attention due to its multiferroic properties. However, the Co site substitution effect on the structural and magnetic properties has rarely been studied in thin film form. In this work, the structural and magnetic properties of Co1-xNixCr2O4 (x = 0, 0.5) epitaxial thin films deposited on MgAl2O4 (100) and MgO (100) substrates to manipulate the nature of strain in the films using pulsed laser deposition (PLD) technique are presented. The epitaxial nature of the films was confirmed through X-ray diffraction (XRD) and Rutherford backscattering spectrometry (RBS) measurements. Raman measurements revealed a disappearance of characteristic A1g and F2g modes of the CoCr2O4 with increase in the Ni content. Atomic force microscopy (AFM) studies show a modification of the surface morphology upon Ni substitution. Magnetic measurements disclose that the ferrimagnetic Curie temperature (Tc) of the CoCr2O4 in thin film grown on MgAl2O4 (100) and MgO (100) substrates were found to be 100.6 +/- 0.5 K and 93.8 +/- 0.2 K, respectively. With Ni substitution the transition temperatures significantly get enhanced from that of CoCr2O4. X-ray photoelectron spectroscopy (XPS) suggests Cr3+ oxidation states in the films, while Co ions are present in a mixed Co2+/Co3+ oxidation state. The substitution of Ni at Co site significantly modifies the line shape of the core level as well as the valence band. Ni ions are also found to be in a mixed 2+/3+ oxidation state. O 1s core level display asymmetry related to possible defects like oxygen vacancies in the films.

cond-mat.mtrl-sci↗

Magneto-dielectric coupling and non-ergodic electrical behaviour in hexagonal Sr0.6Ba0.4MnO3 via local strain driven magnetic ordering

The crystal structure of hexagonal-Sr0.6Ba0.4MnO3 allows various competing superexchange interactions, leading to intriguing magnetic properties. Local structural changes modify overlapping between Mn and oxygen ions with temperature. Calculations based on our model spin-Hamiltonian reveal that the dominant linear antiferromagnetic superexchange interaction between the oxygen-linked Mn4+ ions results in short range correlations (SRC), manifesting a smooth drop in magnetization below 325K. Dominance of superexchange interaction changes its allegiance towards the non-linear oxygen-linked Mn-O-Mn interactions, onsetting long-range correlations (LRC) below 225K. Below the SRC-LRC crossover temperature, electrical response arising from the interacting dipoles exhibits power-law divergent behaviour of relaxation time, upon cooling. Non-ergodic character of the dipole-cluster glass state is examined via the indispensable aging and rejuvenation effects, similar to the spin glasses. Competitive-frustration among spin-exchange and local-strain is reckoned as responsible for the electrical glass origin.

cond-mat.mtrl-sci↗