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Register a new userDynamic atomic reconstruction: how Fe3O4 thin films evade polar catastrophe for epitaxy
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Polar catastrophe at the interface of oxide materials with strongly correlated electrons has triggered a flurry of new research activities. The expectations are that the design of such advanced interfaces will become a powerful route to engineer devices with novel functionalities. Here we investigate the initial stages of growth and the electronic structure of the spintronic Fe3O4/MgO (001) interface. Using soft x-ray absorption spectroscopy we have discovered that the so-called A-sites are completely missing in the first Fe3O4 monolayer. This allows us to develop an unexpected but elegant growth principle in which during deposition the Fe atoms are constantly on the move to solve the divergent electrostatic potential problem, thereby ensuring epitaxy and stoichiometry at the same time. This growth principle provides a new perspective for the design of interfaces.
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Fe3O4 (magnetite) is one of the most elusive quantum materials and at the same time one of the most studied transition metal oxide materials for thin film applications. The theoretically expected half-metallic behavior generates high expectations that it can be used in spintronic devices. Yet, despite the tremendous amount of work devoted to preparing thin films, the enigmatic first order metal-insulator transition and the hall mark of magnetite known as the Verwey transition, is in thin films extremely broad and occurs at substantially lower temperatures as compared to that in high quality bulk single crystals. Here we have succeeded in finding and making a particular class of substrates that allows the growth of magnetite thin films with the Verwey transition as sharp as in the bulk. Moreover, we are now able to tune the transition temperature and, using tensile strain, increase it to substantially higher values than in the bulk.
Magnetite (Fe3O4) thin films on GaAs have been studied with HArd X-ray PhotoElectron Spectroscopy (HAXPES) and low-energy electron diffraction. Films prepared under different growth conditions are compared with respect to stoichiometry, oxidation, and chemical nature. Employing the considerably enhanced probing depth of HAXPES as compared to conventional x-ray photoelectron spectroscopy (XPS) allows us to investigate the chemical state of the film-substrate interfaces. The degree of oxidation and intermixing at the interface are dependent on the applied growth conditions; in particular, we found that metallic Fe, As2O3, and Ga2O3 exist at the interface. These interface phases might be detrimental for spin injection from magnetite into GaAs.
The local epitaxial growth of pulsed laser deposited Ca$_2$MnO$_4$ films on polycrystalline spark plasma sintered Sr$_2$TiO$_4$ substrates was investigated to determine phase formation and preferred epitaxial orientation relationships ($ORs$) for isostructural Ruddlesden-Popper (RP) heteroepitaxy, further developing the high-throughput synthetic approach called Combinatorial Substrate Epitaxy (CSE). Both grazing incidence X-ray diffraction and electron backscatter diffraction (EBSD) patterns of the film and substrate were indexable as single-phase RP-structured compounds. The optimal growth temperature (between 650 $^{circ}$C and 800 $^{circ}$C) was found to be 750 $^{circ}$C using the maximum value of the average image quality (IQ) of the backscattered diffraction patterns. Films grew in a grain-over-grain pattern such that each Ca$_2$MnO$_4$ grain had a single $OR$ with the Sr$_2$TiO$_4$ grain on which it grew. Three primary $ORs$ described 47 out of 49 grain pairs that covered nearly all of RP orientation space. The first $OR$, found for 20 of the 49, was the expected RP unit-cell over RP unit-cell $OR$, expressed as [100][001]$_{film}$||[100][001]$_{sub}$. The other two $ORs$ were essentially rotated from the first by 90$^{circ}$, with one (observed for 17 of 49 pairs) being rotated about the [100] and the other (observed for 10 of 49 pairs) being rotated about the [110] (and not exactly by 90$^{circ}$). These results indicate that only a small number of $ORs$ are needed to describe isostructural RP heteroepitaxy and further demonstrate the potential of CSE in the design and growth of a wide range of complex functional oxides.
We report on the growth of epitaxial Sr2RuO4 films using a hybrid molecular beam epitaxy approach in which a volatile precursor containing RuO4 is used to supply ruthenium and oxygen. The use of the precursor overcomes a number of issues encountered in traditional MBE that uses elemental metal sources. Phase-pure, epitaxial thin films of Sr2RuO4 are obtained. At high substrate temperatures, growth proceeds in a layer-by-layer mode with intensity oscillations observed in reflection high-energy electron diffraction. Films are of high structural quality, as documented by x-ray diffraction, atomic force microscopy, and transmission electron microscopy. The method should be suitable for the growth of other complex oxides containing ruthenium, opening up opportunities to investigate thin films that host rich exotic ground states.
The so-called polar catastrophe, a sudden electronic reconstruction taking place to compensate for the interfacial ionic polar discontinuity, is currently considered as a likely factor to explain the surprising conductivity of the interface between the insulators LaAlO3 and SrTiO3. We applied optical second harmonic generation, a technique that a priori can detect both mobile and localized interfacial electrons, to investigating the electronic polar reconstructions taking place at the interface. As the LaAlO3 film thickness is increased, we identify two abrupt electronic rearrangements: the first takes place at a thickness of 3 unit cells, in the insulating state; the second occurs at a thickness of 4-6 unit cells, i.e., just above the threshold for which the samples become conducting. Two possible physical scenarios behind these observations are proposed. The first is based on an electronic transfer into localized electronic states at the interface that acts as a precursor of the conductivity onset. In the second scenario, the signal variations are attributed to the strong ionic relaxations taking place in the LaAlO3 layer.
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