We have succeeded in preparing high-quality Gd-doped single-crystalline EuO films. Using Eu-distillation-assisted molecular beam epitaxy and a systematic variation in the Gd and oxygen deposition rates, we have been able to observe sustained layer-by-layer epitaxial growth on yttria-stabilized cubic zirconia (001). The presence of Gd helps to stabilize the layer-by-layer growth mode. We used soft x-ray absorption spectroscopy at the Eu and Gd M4,5 edges to confirm the absence of Eu3+ contaminants and to determine the actual Gd concentration. The distillation process ensures the absence of oxygen vacancies in the films. From magnetization measurements we found the Curie temperature to increase smoothly as a function of doping from 70 K up to a maximum of 125 K. A threshold behavior was not observed for concentrations as low as 0.2%.
We have succeeded in growing epitaxial and highly stoichiometric films of EuO on yttria-stabilized cubic zirconia (YSZ) (001). The use of the Eu-distillation process during the molecular beam epitaxy assisted growth enables the consistent achievement of stoichiometry. We have also succeeded in growing the films in a layer-by-layer fashion by fine tuning the Eu vs. oxygen deposition rates. The initial stages of growth involve the limited supply of oxygen from the YSZ substrate, but the EuO stoichiometry can still be well maintained. The films grown were sufficiently smooth so that the capping with a thin layer of aluminum was leak tight and enabled ex situ experiments free from trivalent Eu species. The findings were used to obtain recipes for better epitaxial growth of EuO on MgO (001).
Understanding and manipulating properties emerging at a surface or an interface require a thorough knowledge of structure-property relationships. We report a study of a prototype oxide system, La2/3Sr1/3MnO3 grown on SrTiO3(001), by combining in-situ angle-resolved x-ray photoelectron spectroscopy, ex-situ x-ray diffraction, and scanning transmission electron microscopy/spectroscopy with electric transport measurements. We find that La2/3Sr1/3MnO3 films thicker than 20 unit cells (u.c.) exhibit a universal behavior with no more than one u.c. intermixing at the interface but at least 3 u.c. of Sr segregation near the surface which is (La/Sr)O terminated. The conductivity vs film thickness shows the existence of nonmetallic layers with thickness ~ 6.5 +/- 0.9 u.c., which is independent of film thickness but mainly relates to the deviation of Sr concentration near the surface region. Below 20 u.c., the surface of the films appears mixed (La/Sr)O with MnO2 termination. Decreasing film thickness to less than 10 u.c. leads to the enhanced deviation of chemical composition in the films and eventually drives the film insulating. Our observation offers a natural explanation for the thickness-driven metal-nonmetal transition in thin films based on the variation of film stoichiometry.
Samarium has two stable valence states, 2+ and 3+, which coexist in many compounds forming spatially homogeneous intermediate valence states. We study the valence state of samarium when incorporated in a single crystalline EuO thin film which crystallizes in a $fcc$-structure similar to that of the intermediate valence SmO, but with a larger lattice constant. Due to the increased lattice spacing, a stabilization of the larger Sm$^{2+}$ ion is expected. Surprisingly, the samarium incorporated in Sm$_{mathrm{x}}$Eu$_{mathrm{1-x}}$O thin films shows a predominantly trivalent character, as determined by x-ray photoelectron spectroscopy and magnetometry measurements. We infer that the O$^{2-}$ ions in the EuO lattice have enough room to move locally, so as to reduce the Sm-O distance and stabilize the Sm$^{3+}$ valence.
The electronic and magnetic properties of ferromagnetic doped manganites are investigated by means of model tight-binding and textit{ab initio} self-interaction corrected local spin density approximation calculations. It is found that the surface alone by breaking the cubic symmetry induces a difference in the occupation of the two $e_{g}$ orbitals at the surface. With textit{ab initio} calculations we found surface localisation of one orbital and hence a change in the Mn valency from four in the bulk to three at the sub-surface. Different surface or disordered interface induced localisation of the orbitals are considered too with respect to the nature and the strength of the magnetic exchange coupling between the surface/interface and the bulk-like region.
Highly oriented polycrystalline SSMO thin films deposited on single crystal substrates by ultrasonic nebulized spray pyrolysis have been studied. The film on LAO is under compressive strain while LSAT and STO are under tensile strain. The presence of a metamagnetic state akin to cluster glass formed due to coexisting FM and antiferromagnetic/charge order (AFM/CO) clusters. All the films show colossal magnetoresistance but its temperature and magnetic field dependence are drastically different. In the lower temperature region the magnetic field dependent isothermal resistivity also shows signature of metamagnetic transitions. The observed results have been explained in terms of the variation of the relative fractions of the coexisting FM and AFM/CO phases as a function of the substrate induced strain and oxygen vacancy induced quenched disorder.