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In the present work, interfacial magnetism at metal organic interface is probed using an isotope sensitive interface resolved nuclear resonance scattering technique which is made depth selective under x-rays standing wave conditions. Using GIWAXS and GINRS measurements, this study evidences the presence of symmetry-based PMA which appears at a lower thickness of Fe having distortion in cubic symmetry and disappears at a higher thickness of Fe as its cubic symmetry retains. The non-zero value of quadrupole splitting evidences the strain at the interfacial region which on increasing thickness of Fe relaxes. The diffusion of Fe is traced using XRF and NRR, deep penetration of Fe in Alq3 layer due to soft nature of the organic film is obtained. This thickness-dependent study enables us to understand the magnetic behavior of buried ferromagnetic metal in the vicinity of organic molecules.

Interfaces in FeCoB/MgO/FeCoB magnetic tunnel junction play a vital role in controlling their magnetic and transport properties for various applications in spintronics and magnetic recording media. In this work, interface structures of a few nm thick FeCoB layers in FeCoB/MgO and MgO/FeCoB bilayers are comprehensively studied using x-ray standing waves (XSW) generated by depositing bilayers between Pt waveguide structures. High interface selectivity of nuclear resonance scattering (NRS) under the XSW technique allowed measuring structure and magnetism at the two interfaces, namely FeCoB-on-MgO and MgO-on-FeCoB, yielding an interesting result that electron density and hyperfine fields are not symmetric at both interfaces. The formation of a high-density FeCoB layer at the MgO/FeCoB (FeCoB-on-MgO) interface with an increased hyperfine field (~34.65 T) is attributed to the increasing volume of FeCo at the interface due to boron diffusion from 57FeCoB to the MgO layer. Furthermore, it caused unusual angular-dependent magnetic properties in MgO/FeCoB bilayer, whereas FeCoB/MgO is magnetically isotropic. In contrast to the literature, where the unusual angular dependent in FeCoB based system is explained in terms of in-plane magnetic anisotropy, present findings attributed the same to the interlayer exchange coupling between bulk and interface layer within the FeCoB layer.

Interface magnetism and topological structure of Fe on organic semiconductor film (Alq3) have been studied and compared with Fe film deposited directly on Si (100) substrate. To get information on the diffused Fe layer at the Fe/Alq3 interface, grazing incident nuclear resonance scattering (GINRS) measurements are made depth selective by introducing a 95% enriched thin 57Fe layer at the Interface and producing x-ray standing wave within the layered structure. Compared with Fe growth on Si substrate, where film exhibits a hyperfine field value of 32 T (Bulk Fe), a thick Fe- Alq3 interface has been found with reduced electron density and hyperfine fields providing evidence of deep penetration of Fe atoms into Alq3 film. Due to the soft nature of Alq3, Fe moments relax in the film plane. At the same time, Fe on Si has a resultant ~43 deg out-of-plane orientation of Fe moments at the Interface due to the stressed and rough Fe layer near Si. The evolution of magnetism at the Fe-Alq3 Interface is monitored using in-situ magneto-optical Kerr effect (MOKE) during the growth of Fe on the Alq3 surface and small-angle x-ray scattering (SAXS) measurements. It is found that the Fe atom tries to organize into clusters to minimize their surface/interface energy. The origin of the 2.4 nm thick magnetic dead layer at the Interface is attributed to the small Fe clusters of paramagnetic or superparamagnetic nature. The present work provides an understanding of interfacial magnetism at metal-organic interfaces and the topological study using the GI-NRS technique, which is made depth selective to probe magnetism of the diffused ferromagnetic layer, which is otherwise difficult for lab-based techniques.

The effect of the saturation field on the magnetization reversal of FePt(L10)/FeCo/CoO/FeCo multilayer (ML) has been investigated to understand the origin of asymmetric magnetization reversal and its correlation with exchange bias (EB). In the ML structure, the bottom FeCo layer is coupled to the hard FePt(L10) layer, and the top FeCo layer is comparatively free due to the relatively more distance from it. The ML has been deposited under UHV conditions and characterized at each stage of growth using magneto-optical Kerr effect and x-ray reflectivity techniques. Magnetization reversal is further studied through domain imaging using the Kerr microscopy technique. The experimental findings reveal that ML exhibits asymmetrical magnetization reversal for a certain range of azimuthal angles for both 1.5kOe and 50kOe saturation fields; however, this angular range of asymmetry decreases with the increase in the saturation field. Furthermore, EB was absent at the low saturation field, whereas, EB, in addition to asymmetry, is observed at the large saturation field. The origin of asymmetry is attributed to non-collinearity between magnetic anisotropy axes of both FeCo layers. It results from the proximity effect through short-range Heisenberg exchange interaction via the CoO barrier layer. On the other hand, EB arises due to unidirectional anisotropy induced in the FePt layer due to the high saturation field. It is further proposed that asymmetry would disappear when unidirectional anisotropy is strong enough to align both the FeCo layers in the saturation direction leading to loss of the non-collinearity between them., Comment: 16 pages, 8 figures, 1 table

Magnetoelastic and magnetoelectric coupling in the artificial multiferroic heterostructures facilitate valuable features for device applications such as magnetic field sensors and electric write magnetic-read memory devices. In a ferromagnetic/ferroelectric heterostructures, the strain mediated coupling exploits piezoelectricity/electrostriction in ferroelectric phase and magnetostriction/piezomagnetism in ferromagnetic phase. Such verity of these combined effect can be manipulated by an external perturbation, such as electric field, temperature or magnetic field. Here, we demonstrate the remote-controlled tunability of these effects under the visible, coherent and polarized light. The combined surface and bulk magnetic study of domain-correlated Ni/BaTiO3 heterostructure reveals that the system is strong sensitive about the light illumination via the combined effect of converse piezoelectric, magnetoelastic coupling and converse magnetostriction. Well-defined ferroelastic domain structure is fully transferred from a tetragonal ferroelectric to magnetostrictive layer via interface strain transfer during the film growth. The visible light illumination is used to manipulate the original ferromagnetic microstructure by the light-induced domain wall motion in ferroelectric, consequently the domain wall motion in the ferromagnetic layer. Our findings mimic the attractive remote-controlled ferroelectric random-access memory write and magnetic random-access memory read application scenarios, hence, can be proven as a novel perspective for room temperature device applications., Comment: 35 pages, 7 figures

High temperature one-dimensional (1D) ferromagnetic (FM) chains in Ca3Co2O6 spin system are subjected to a magnetic field and temperature induced first order phase transition (FOPT) to 3D ferrimagnetic (FIM) ground state with decrease in temperature (T). Weak-FM interaction of third nearest-neighbor(nn) interchain removes the frustration effect arising from antiferromagnetic (AFM) interactions of first-nn and second-nn interchains in the underlying triangular-lattice resulting a 3D FIM ordering of 1D FM chains at low T. However, hindered kinetics of FOPT partially masks this tranformation giving rise to coexistence of non-interacting 1D FM chains with 3D-FIM state at low-T. The existence of all these couplings is further confirmed here by random substitution of S = 5/2 magnetic-impurity into the spin chain of original system. It reveals weakening of FM interactions of both intrachain and third-nn surrounding chains respectively without significant modulation in the AFM coupling of first-nn and second-nn interchains. Thus, influence of AFM interactions is enhanced as compared to effective FM coupling with increase of S = 5/2 impurity content resulting instability of 3D long-range FIM state at low-T.

We observed that close to a Mott transition, over a small temperature range, the predominance of slow relaxations leads to decoupling of electrons from the thermal bath. This has been established by observation of large deviation of the thermal noise in the films of Mott system $NdNiO_{3}$ from the canonical Johnson-Nyquist value of $4k_{B}TR$ close to the transition. It is suggested that such a large noise arise from small isolated pockets of nanometric metallic phases (estimated size $\sim$ 15-20 nm) within the insulating phase with the charging energy as the control parameter., Comment: 27 pages with Supplementary, In revised version discussion updated, New references

Alpha-Fe2O3 and alpha-Cr2O3 has been mechanical alloyed to prepare Fe1-xCrxO3 oxides for x = 0.2-0.8. Synchrotron X-ray diffraction and Raman spectra have shown inhomogeneous structure of {\alpha}-Fe2O3 and {\alpha}-Cr2O3 phases in as-alloyed samples. The as-alloyed samples have shown soft ferromagnetic properties with signature of two Morin transitions. The heat treatment of as-alloyed samples has homogenized structure and successfully incorporated the Cr atoms into the lattice sites of Fe atoms in {\alpha}-Fe2O3. The magnetic and electrical properties have been modified in the heat treated samples. For example, canted antiferromagnetic order has been appeared as an effect of heat treatment, irrespective of the Cr content in Fe1-xCrxO3. The magnetic field induced spin flop transition has been observed at a critical magnetic field that depends on Cr content in the system. The M\"ossbauer spectrum at room temperature has been fitted with two sextets. The variation of M\"ossbauer parameters suggest a distribution of magnetic spin order between Fe and Cr ions in the rhombohedral structure of Fe1-xCrxO3. The electrical conductivity, derived from current-voltage characteristics of the heat treated samples, has been enhanced by increasing Cr content in alpha-Fe2O3 structure. The experimental results have been explained based on the theoretical models available in literature.

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

We studied the structural and magnetic properties of \FeC~thin films deposited by co-sputtering of Fe and C targets in a direct current magnetron sputtering (dcMS) process at a substrate temperature (\Ts) of 300, 523 and 773\,K. The structure and morphology was measured using x-ray diffraction (XRD), x-ray absorption near edge spectroscopy (XANES) at Fe $L$ and C $K$-edges and atomic/magnetic force microscopy (AFM, MFM), respectively. An ultrathin (3\,nm) $^{57}$\FeC~layer, placed between relatively thick \FeC~layers was used to estimate Fe self-diffusion taking place during growth at different \Ts~using depth profiling measurements. Such $^{57}$\FeC~layer was also used for $^{57}$Fe conversion electron M\"{o}ssbauer spectroscopy (CEMS) and nuclear resonance scattering (NRS) measurements, yielding the magnetic structure of this ultrathin layer. We found from XRD measurements that the structure formed at low \Ts~(300\,K) is analogous to Fe-based amorphous alloy and at high \Ts~(773\,K), pre-dominantly a \tifc~phase has been formed. Interestingly, at an intermediate \Ts~(523\,K), a clear presence of \tefc~(along with \tifc~and Fe) can be seen from the NRS spectra. The microstructure obtained from AFM images was found to be in agreement with XRD results. MFM images also agrees well with NRS results as the presence of multi-magnetic components can be clearly seen in the sample grown at \Ts~= 523\,K. The information about the hybridization between Fe and C, obtained from Fe $L$ and C $K$-edges XANES also supports the results obtained from other measurements. In essence, from this work, experimental realization of \tefc~has been demonstrated. It can be anticipated that by further fine-tuning the deposition conditions, even single phase \tefc~phase can be realized which hitherto remains an experimental challenge., Comment: 11 pages, 9 figures

Epitaxial Fe4N thin films grown on lattice-matched LaAlO3 (LAO) substrate using sputtering and molecular beam epitaxy techniques have been studied in this work. Within the sputtering process, films were grown with conventional direct current magnetron sputtering (dcMS) and for the first time, using a high power impulse magnetron sputtering (HiPIMS) process. Surface morphology and depth profile reveal that HiPIMS deposited film has the lowest roughness, the highest packing density and the sharpest interface. La from the LAO substrate and Fe from the film interdiffuse and forms an undesired interface spreading to an extent of about 10-20 nm. In the HiPIMS process, layer by layer type growth leads to a globular microstructure which restricts the extent of the interdiffused interface. Such substrate-film interactions and microstructure play a vital role in affecting the electronic hybridization and magnetic properties of Fe4N films. The magnetic moment (Ms) was compared using bulk, element-specific and magnetic depth profiling techniques. We found that Ms was the highest when the thickness of the interdiffused layer was lowest and only be achieved in the HiPIMS grown samples. Presence of small moment at the N site was also evidenced by element-specific x-ray circular dichroism measurement in HiPIMS grown sample. A large variation in the Ms values of Fe4N found in the experimental works carried out so far could be due to such interdiffused layer which is generally not expected to form in otherwise stable oxide substrate. In addition, a consequence of substrate-film interdiffusion and microstructure results in different kinds of different kind of magnetic anisotropies in films grown using different techniques., Comment: 8 pages, 8 figures, Supplementary Material

We studied the structural and magnetic properties of \textit{in-situ} grown iron mononitride (FeN) thin films. Initial stages of film growth were trapped utilizing synchrotron based soft x-ray absorption near edge spectroscopy (XANES) at the N $K$-edge and nuclear resonant scattering (NRS). Films were grown using dc-magnetron sputtering, separately at the experimental stations of SXAS beamline (BL01, Indus 2) and NRS beamline (P01, Petra III). It was found that the initial stages of film growth differs from the bulk of it. Ultrathin FeN films, exhibited larger energy separation between the t$_{2g}$ and e$_g$ features and an intense e$_g$ feature in the N $K$-edge pattern. This indicates that a structural transition is taking place from the rock-slat (RS)-type FeN to zinc-blende(ZB)-type FeN when the thickness of films increases beyond 5\,nm. The behavior of such N $K$-edge features correlates very well with the emergence of a magnetic component appearing in the NRS pattern at 100\,K in ultrathin FeN films. Combining the \textit{in-situ} XANES and NRS measurements, it appears that initial FeN layers grow in RS-type structure having a magnetic ground state. Subsequently, the structure changes to ZB-type which is known to be non-magnetic. Observed results help in resolving the long standing debate about the structure and the magnetic ground state of FeN., Comment: 9 pages, 5 figures

In this work, we studied the pathways for formation of stoichiometric \tcn~thin films. Polycrystalline and epitaxial \tcn~films were prepared using reactive direct current magnetron (dcMS) sputtering technique. A systematic variation in the substrate temperature (\Ts) during the dcMS process reveals that the lattice parameter (LP) decreases as \Ts~increases. We found that nearly stoichiometric \tcn~films can be obtained when \Ts~= 300\,K. However, they emerge from the transient state of Co target ($\phi$3\,inch). By reducing the target size to $\phi$1\,inch, now the \tcn~phase formation takes place from the metallic state of Co target. In this case, LP of \tcn~film comes out to be $\sim$99\p~of the value expected for \tcn. This is the largest value of LP found so far for \tcn. The pathways achieved for formation of polycrystalline \tcn~were adopted to grow an epitaxial \tcn~film, which shows four fold magnetic anisotropy in magneto-optic Kerr effect measurements. Detailed characterization using secondary ion mass spectroscopy indicates that N diffuses out when \Ts~is raised even to 400\,K. Measurement of electronic structure using x-ray photoelectron spectroscopy and x-ray absorption spectroscopy further confirms it. Magnetization measurements using bulk magnetization and polarized neutron reflectivity show that the saturation magnetization of stoichiometric \tcn~film is even larger than pure Co. Since all our measurements indicated that N could be diffusing out, when \tcn~films are grown at high \Ts, we did actual N self-diffusion measurements in a CoN sample and found that N self-diffusion was indeed substantially higher. The outcome of this work clearly shows that the \tcn~films grown prior to this work were always N deficient and the pathways for formation of a stoichiometric \tcn~have been achieved., Comment: 12 pages, 18 figures

Enhanced magnetic moment and coercivity in SrRuO3 thin films are significant issues for advanced technological usages and hence are researched extensively in recent times. Most of the previous reports on thin films with enhanced magnetic moment attributed the high spin state for the enhancement. Our magnetization results show high magnetic moment of 3.3 Bohr-magnetron/Ru ion in the epitaxial thin films grown on LSAT substrate against 1.2 Bohr-magnetron/Ru ion observed in bulk compound. Contrary to the expectation the Ru ions are found to be in low spin state and the orbital moment is shown to be contributing significantly in the enhancement of magnetic moment. We employed x-ray absorption spectroscopy and resonant valance band spectroscopy to probe the spin state and orbital contributions in these films. The existence of strong spin-orbit coupling responsible for the de-quenching of the 4d orbitals is confirmed by the observation of the non-statistical large branching ratio at the Ru M2,3 absorption edges. The relaxation of orbital quenching by strain engineering provides a new tool for enhancing magnetic moment. Strain disorder is shown to be an efficient mean to control the spin-orbit coupling., Comment: 10 pages, 6 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 report here sign reversal and tunability of exchange bias in AuFe cosputtered films of thickness about 63 nm. As deposited film exhibits exchange bias effect at room temperature without external triggering field and its magnitude increases gradually with decrease in temperature down to 5 K. Upon irradiation with 100 MeV Au9+ ions at a fluence of 5*1013 ions/cm2, hysteresis loop shifts completely from origin towards positive field side at room temperature and reverses sign when temperature is reduced to 5 K as studied by SQUID magnetometry. A well defined uniaxial magnetic anisotropy has been seen by magneto optical Kerr effect (MOKE) in as deposited film as well as in irradiated one. The results are explained on the basis of stress induced magnetic anisotropy in thin films.

Mossbauer analysis is carried out on CZTS samples, subjected to a low temperature processing at 3000C (S1) and high temperature processing at 5500C under sulfur environment (S2). Loss of Sn is observed in sample S2 due to high temperature thermal treatment.The isomer shifts obtained in the Mossbauer spectra confirms the existence of Sn at its 4+ valance state in both the samples. Relatively high quadriple splitting is observed in S1 with respect to S2, suggesting dislocations and crystal distortion present in S1, which are reduced drastically by high temperature annealed S2 sample. The fabricated solar cell with S1 and S2 absorbers showed significant improvement in efficiency from ~0.145% to ~1%. The presence of excess Sn in S1 allows enhanced recombination and the diode ideality factor shows larger value of 4.23 compared to 2.17 in case of S2. The experiments also validate the fact that S1 with Sn rich configuration shows lower acceptor carrier concentration as compared to S2 because of enhanced compensating defects in S1., Comment: 21 pages, 8 figures, 5 tables. Submitted to Materials Chemistry and Physics Journal

We have carried out systematic temperature-dependent neutron diffraction measurements in conjunction with dielectric spectroscopy from 6 to 300 K for sodium niobate based compounds (1-x) NaNbO3 -xBaTiO3 (NNBTx). The dielectric constant is measured both as a function of temperature and frequency. It shows an anomaly at different temperatures in cooling and heating cycles and exhibits a large thermal hysteresis of 150 K for the composition x=0.03. The dielectric constant is found to be dispersive in nature and suggests a relaxor ferroelectric behavior. In order to explore structural changes as a function of temperature, we analyzed the powder neutron diffraction data for the composition x=0.03 and 0.05, respectively. Drastic changes are observed in the powder profiles near 30.6{\deg}, 32.1{\deg} and 34.6{\deg} in the diffraction pattern below 200 K during cooling and above 190 K in heating cycles, respectively.The disappearance of superlattice reflection and splitting in main perovskite peaks provide a signature for structural phase transition. We observed stabilization of a monoclinic phase (Cc) at low temperature. This monoclinic phase is believed to provide a flexible polarization rotation and considered to be directly linked to the high performance piezoelectricity in materials. The thermal hysteresis for composition x=0.03 is larger than x=0.05. This suggests that addition of BaTiO3 in NaNbO3 suppresses the thermal hysteresis. It is also observed that the structural phase transition temperature decreases on increasing dopant concentration., Comment: 16 Pages, 6 Figures

FeGa3 is a well known d-p hybridization induced intermetallic bandgap semiconductor. In this work, we present the experimental and theoretical results on the effect of Al substitution in FeGa3, obtained by x-ray diffraction (XRD), temperature dependent resistance measurement, room temperature Mossbauer measurements and density functional theory based electronic structure calculations. It is observed that upto x = 0.178 in Fe(AlxGa1-x)3, which is the maximum range studied in this work, Al substitution reduces the lattice parameters 'a' and 'c' preserving the parent tetragonal P42/mnm crystal structure of FeGa3. The bandgap of Fe(AlxGa1-x)3 for x = 0.178 is reduced by ~ 24% as compared to FeGa3. Rietveld refinement of the XRD data shows that the Al atoms replace Ga atoms located at the 8j sites in FeGa3. A comparison of the trends of the lattice parameters and energy bandgap observed in the calculations and the experiments also confirms that Al primarily replaces the Ga atoms in the 8j site., Comment: 6 pages, 5 figures, 3 tables

Polycrystalline HoSn1.1Ge0.9 and DySn1.1Ge0.9 compounds have been studied by means of different experimental probes. Both the compounds are antiferromagnetic and show metamagnetic transition at low temperatures. HoSn1.1Ge0.9 shows a sign change in magnetocaloric effect (MCE) and magnetoresistance (MR) with field, which is attributed to the metamagnetic transition. DySn1.1Ge0.9 shows characteristics of a typical antiferromagnet, as evidenced by magnetization, MCE and MR data. 119Sn M\"ossbauer studies show hyperfine splitting at low temperatures, consistent with magnetization data. Thermoelectric power and resistivity measurements reveal metallic behavior in these compounds. Magnetic, magnetocaloric and the magnetoresistance data clearly show that the antiferromagnetic coupling in DySn1.1Ge0.9 is stronger than in HoSn1.1Ge0.9., Comment: 14 pages, 9 figures