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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.

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 ($\epsilon_1$) and the optical conductivity ($\sigma_1$) 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 $\sigma_1$ is maximum and $\epsilon_1$ 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 $\sigma_1$ reduces and $\epsilon_1$ 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., Comment: 18 pages, 6 figures

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., Comment: 28,13

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., Comment: 11 pages, 3 figures

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., Comment: 14 pages, 10 figures

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} $)., Comment: 8 pages, 3 figures

Ferromagnetic insulators (FM-Is) are the materials of interest for new generation quantum electronic applications. Here, we have investigated the physical observables depicting FM-I ground states in epitaxial Sm$ _{2} $NiMnO$ _{6} $ (SNMO) double perovskite thin films fabricated under different conditions to realize different level of Ni/Mn anti-site disorders (ASDs). The presence of ASDs immensely influence the characteristic magnetic and anisotropy behaviors in SNMO system by introducing short scale antiferromagnetic interactions in predominant long range FM ordered host matrix. Charge disproportion between cation sites in form of $ Ni^{2+}+Mn^{4+} \longrightarrow Ni^{3+}+Mn^{3+} $, causes mixed valency in both Ni and Mn species, which is found insensitive to ASD concentrations. Temperature dependent photo emission, photo absorption measurements duly combined with cluster model configuration interaction simulations, suggest that the eigenstates of Ni and Mn cations can be satisfactorily described as a linear combination of the unscreened $ d^{n} $ and screened $ d^{n+1} \underline{L} $ ($ \underline{L} $: O 2\textit{p} hole) states. The electronic structure across the Fermi level (E$ _{F} $) exhibits closely spaced Ni $ 3d $, Mn $ 3d $ and O $ 2p $ states. From occupied and unoccupied bands, estimated values of the Coulomb repulsion energy ($ U $) and ligand to metal charge transfer energy ($ \Delta $), indicate charge transfer insulating nature, where remarkable modification in Ni/Mn $ 3d $ - O $ 2p $ hybridization takes place across the FM transition temperature. Existence of ASD broadens the Ni, Mn $ 3d $ spectral features, whereas spectral positions are found to be unaltered. Hereby, present work demonstrates SNMO thin film as a FM-I system, where FM state can be tuned by manipulating ASD in the crystal structure, while I state remains intact., Comment: 21 pages, 9 figures, and supplemental information

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 ($\Delta_{ct}$) with the La substitution., Comment: submitted

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., Comment: 14 pages, 8 figures, and Supplementary Information

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 {\alpha} 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., Comment: 26 pages, 9 figures

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 ({\alpha}) by applying selective positive and negative electric fields in a non-volatile manner. The retention of two stable states of {\alpha} 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., Comment: 19 pages, 5 figures

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., Comment: 7 pages, 10 figures

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.

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., Comment: 30 pages, 8 figures

The present study reports on the structural and magnetic phase transitions in Pr-doped polycrystalline Tb0.6Pr0.4MnO3, using high-resolution neutron powder diffraction (NPD) collected at SINQ spallation source (PSI), to emphasize the suppression of the sinusoidal magnetic structure of pure TbMnO3 and the evolution to a collinear A-type antiferromagnetic ordering. The phase purity, Jahn-Teller distortion, and one-electron bandwidth for eg orbital of Mn3+ cation have been calculated for polycrystalline Tb0.6Pr0.4MnO3, in comparison to the parent materials TbMnO3 and PrMnO3, through the Rietveld refinement study from X-ray diffraction data at room temperature. The temperature-dependent zero field-cooled and field-cooled dc magnetization study at low temperature down to 5 K reveals a variation in the magnetic phase transition due to the effect of Pr3+ substitution at the Tb3+ site, which gives the signature of the antiferromagnetic nature of the sample, with a weak ferromagnetic component at low temperature induced by an external magnetic field. The field-dependent magnetization study at low temperatures gives the weak coercivity having the order of 2 kOe, which is expected due to canted-spin arrangement or ferromagnetic nature of Terbium ordering. The NPD data for Tb0.6Pr0.4MnO3 confirms that the nuclear structure of the synthesized sample maintains its orthorhombic symmetry down to 1.5 K. Also, the magnetic structures have been solved at 50 K, 25 K, and 1.5 K through the NPD study, which shows A-type antiferromagnetic spin arrangement., Comment: 21 Pages, 8 Figures, 7 Tables

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., Comment: 25 pages, 7 figures and supplementary information

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., Comment: 26 pages, 6 figures

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)., Comment: 23 pages, 9 figures

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., Comment: 41 pages, 16 figures, article

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., Comment: 20 pages, 6 figures, 32 references. arXiv admin note: substantial text overlap with arXiv:1807.01303

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., Comment: 19 pages, 6 figures

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 $\pi^{\ast}$ and the $\sigma^{\ast}$ states (which are O 2$\it{p}$ hybridized V 3$\it{d}$ $e_g^{\pi}$ and $e_g^{\sigma}$ 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., Comment: 7 pages and 4 figures

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., Comment: 15 pages, 3 figures

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.

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., Comment: 26 Pages, 9 Figures

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., Comment: 7 pages, 12 figures

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.

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.

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., Comment: 15 pages, 4 figures, 1 table, and 28 references

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., Comment: Page 20 and 6 figures

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 N\'eel 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), $\Delta T \sim 110$ K in presence of $\mu_0H$ = 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 $\AA$. 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$_{3}$., Comment: 11 pages, 8 figures

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., Comment: 28 pages, 10 figures, Journal of Applied Physics 2017

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., Comment: Latest research work in Revtex format including 4 pages and 5 figures

We report the existence of ferromagnetic correlations (FMC) in paramagnetic (PM) matrix of cubic La1-xSrxMnO3-{\delta} (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., Comment: Accepted in Physica status solidi (b), 19 Page, 5 figures

Structural phase transition studies employing low-temperature transmission electron microscopy, and low-temperature x-ray diffraction have been carried out on nearly stoichiometric ({\delta}=0.01) and off-stoichiometric ({\delta}=0.12) versions of La0.2Sr0.8MnO3-{\delta} manganite. The nearly stoichiometric La0.2Sr0.8MnO3-{\delta} under goes a cubic to Jahn-Teller distorted C-type antiferromagnetic tetragonal phase-transition at 260K. For off-stoichiometric La0.2Sr0.8MnO3-{\delta} 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 ({\rho}) on temperature (T) i.e. {\rho}=C.T-{\alpha} has been realized. This has been attributed to multistep inelastic tunneling through channels involving localized states around oxygen vacancy sites., Comment: 26 pages, 5 figures