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Register a new userImpact of strain and morphology on magnetic properties of Fe$_3$O$_4$/NiO bilayers grown on Nb:SrTiO$_3$(001) and MgO(001)
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We present a comparative study on the morphology and structural as well as magnetic properties of crystalline Fe$_3$O$_4$/NiO bilayers grown on both MgO(001) and SrTiO$_3$(001) substrates by reactive molecular beam epitaxy. These structures are investigated by means of x-ray photoelectron spectroscopy, low energy electron diffraction, x-ray reflectivity and diffraction as well as vibrating sample magnetometry. While the lattice mismatch of NiO grown on MgO(001) is only 0.8%, it is exposed to a lateral lattice mismatch of -6.9% if grown on SrTiO$_3$. In the case of Fe$_3$O$_4$, the misfit strain on MgO(001) and SrTiO$_3$(001) amounts to 0.3% and -7.5%, respectively. To clarify the relaxation process of the bilayer system, the film thicknesses of the magnetite and nickel oxide films have been varied between 5 and 20nm. While NiO films are well ordered on both substrates, Fe$_3$O$_4$ films grown on NiO/SrTiO$_3$ exhibit a higher surface roughness as well as lower structural ordering compared to films grown on NiO/MgO. Further, NiO films grow pseudomorphic in the investigated thickness range on MgO substrates without any indication of relaxation, whereas on SrTiO$_3$ the NiO films show strong strain relaxation. Fe$_3$O$_4$ films exhibit also strong relaxation even for films of 5nm thickness on both NiO/MgO as well as on NiO/SrTiO$_3$. The magnetite layers on both substrates show a fourfold magnetic in-plane anisotropy with magnetic easy axes pointing in $leftlangle100rightrangle$ directions. The coercive field is strongly enhanced for magnetite grown on NiO/SrTiO$_3$ due to higher density of structural defects, compared to magnetite grown on NiO/MgO.
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We study the underlying chemical, electronic and magnetic properties of a number of magnetite based thin films. The main focus is placed onto NiO/Fe$_3$O$_4$(001) bilayers grown on MgO(001) and Nb-SrTiO$_3$(001) substrates. We compare the results with those obtained on pure Fe$_3$O$_4$(001) thin films. It is found that the magnetite layers are oxidized and Fe$^{3+}$ dominates at the surfaces due to maghemite ($gamma$-Fe$_2$O$_3$) formation, which decreases with increasing magnetite layer thickness. From a layer thickness of around 20 nm on the cationic distribution is close to that of stoichiometric Fe$_3$O$_4$. At the interface between NiO and Fe$_3$O$_4$ we find the Ni to be in a divalent valence state, with unambiguous spectral features in the Ni 2p core level x-ray photoelectron spectra typical for NiO. The formation of a significant NiFe$_2$O$_4$ interlayer can be excluded by means of XMCD. Magneto optical Kerr effect measurements reveal significant higher coercive fields compared to magnetite thin films grown on MgO(001), and a 45$^{circ}$ rotated magnetic easy axis. We discuss the spin magnetic moments of the magnetite layers and find that the moment increases with increasing thin film thickness. At low thickness the NiO/Fe$_3$O$_4$ films grown on Nb-SrTiO$_3$ exhibits a significantly decreased spin magnetic moments. A thickness of 20 nm or above leads to spin magnetic moments close to that of bulk magnetite.
Crystalline Fe3O4/NiO bilayers were grown on MgO(001) substrates using reactive molecular beam epitaxy to investigate their structural properties and their morphology. The film thickness either of the Fe3O4 film or of the NiO film has been varied to shed light on the relaxation of the bilayer system. The surface properties as studied by x-ray photo electron spectroscopy and low energy electron diffraction show clear evidence of stoichiometric well-ordered film surfaces. Based on the kinematic approach x-ray diffraction experiments were completely analyzed. As a result the NiO films grow pseudomorphic in the investigated thickness range (up to 34nm) while the Fe3O4 films relax continuously up to the thickness of 50nm. Although all diffraction data show well developed Laue fringes pointing to oxide films of very homogeneous thickness, the Fe3O4-NiO interface roughens continuously up to 1nm root-mean-square roughness with increasing NiO film thickness while the Fe3O4 surface is very smooth independent on the Fe3O4 film thickness. Finally, the Fe3O4-NiO interface spacing is similar to the interlayer spacing of the oxide films while the NiO-MgO interface is expanded.
By combining ab initio simulations including an on-site Coulomb repulsion term and Boltzmann theory, we explore the thermoelectric properties of (LaNiO$_3$)$_n$/(LaAlO$_3$)$_n$(001) superlattices ($n=1,3$) and identify a strong dependence on confinement, spacer thickness, and epitaxial strain. While the system with $n=3$ shows modest values of the Seebeck coefficient and power factor, the simultaneous reduction of the LaNiO$_3$ region and the LaAlO$_3$ spacer thickness to single layers results in a strong enhancement, in particular of the in-plane values. This effect can be further tuned by using epitaxial strain as control parameter: Under tensile strain corresponding to the lateral lattice constant of SrTiO$_3$ we predict in- and cross-plane Seebeck coefficients of $pm 600$ $mu$V/K and an in-plane power factor of $11$ $mu$W/K$^2$cm for an estimated relaxation time of $tau = 4$ fs around room temperature. These values are comparable to some of the best performing oxide systems such as La-doped SrTiO$_3$ or layered cobaltates and are associated with the opening of a small gap ($0.29$ eV) induced by the concomitant effect of octahedral tilting and Ni-site disproportionation. This establishes oxide superlattices at the verge of a metal-to-insulator transition driven by confinement and strain as promising candidates for thermoelectric materials.
The interface structure of Fe/MgO(100) magnetic tunnel junctions predicted by density functional theory (DFT) depends significantly on the choice of exchange and correlation functional. Bader analysis reveals that structures obtained by relaxing the cell with the local spin-density approximation (LSDA) display a different charge transfer than those relaxed with the generalized gradient approximation (GGA). As a consequence, the electronic transport is found to be extremely sensitive to the interface structure. In particular, the conductance for the LSDA-relaxed geometry is about one order of magnitude smaller than that of the GGA-relaxed one. The high sensitivity of the electronic current to the details of the interface might explain the discrepancy between the experimental and calculated values of magnetoresistance.
A comprehensive bulk and surface investigation of high-quality In$_2$O$_3$(001) single crystals is reported. The transparent-yellow, cube-shaped single crystals were grown using the flux method. Inductively coupled plasma mass spectrometry (ICP-MS) reveals small residues of Pb, Mg, and Pt in the crystals. Four-point-probe measurements show a resistivity of 2.0 $pm$ 0.5 $times$ 10$^5$ {Omega} cm, which translates into a carrier concentration of $approx$10$^{12}$ cm$^{-3}$. The results from x-ray diffraction (XRD) measurements revise the lattice constant to 10.1150(5) {AA} from the previously accepted value of 10.117 {AA}. Scanning tunneling microscopy (STM) images of a reduced (sputtered/annealed) and oxidized (exposure to atomic oxygen at 300 {deg}C) surface show a step height of 5 {AA}, which indicates a preference for one type of surface termination. The surfaces stay flat without any evidence for macroscopic faceting under any of these preparation conditions. A combination of low-energy ion scattering (LEIS) and atomically resolved STM indicates an indium-terminated surface with small islands of 2.5 {AA} height under reducing conditions, with a surface structure corresponding to a strongly distorted indium lattice. Scanning tunneling spectroscopy (STS) reveals a pronounced surface state at the Fermi level ($E_F$). Photoelectron spectroscopy (PES) shows additional, deep-lying band gap states, which can be removed by exposure of the surface to atomic oxygen. Oxidation also results in a shoulder at the O 1s core level at a higher binding energy, possibly indicative of a surface peroxide species. A downward band bending of 0.4 eV is observed for the reduced surface, while the band bending of the oxidized surface is of the order of 0.1 eV or less.
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