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Register a new userNovel Multifunctional Materials Based on Oxide Thin Films and Artificial Heteroepitaxial Multilayers
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Transition metal oxides show fascinating physical properties such as high temperature superconductivity, ferro- and antiferromagnetism, ferroelectricity or even multiferroicity. The enormous progress in oxide thin film technology allows us to integrate these materials with semiconducting, normal conducting, dielectric or non-linear optical oxides in complex oxide heterostructures, providing the basis for novel multi-functional materials and various device applications. Here, we report on the combination of ferromagnetic, semiconducting, metallic, and dielectric materials properties in thin films and artificial heterostructures using laser molecular beam epitaxy. We discuss the fabrication and characterization of oxide-based ferromagnetic tunnel junctions, transition metal-doped semiconductors, intrinsic multiferroics, and artificial ferroelectric/ferromagetic heterostructures - the latter allow for the detailed study of strain effects, forming the basis of spin-mechanics. For characterization we use X-ray diffraction, SQUID magnetometry, magnetotransport measurements, and advanced methods of transmission electron microscopy with the goal to correlate macroscopic physical properties with the microstructure of the thin films and heterostructures.
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Recent advances in high-throughput experimentation for combinatorial studies have accelerated the discovery and analysis of materials across a wide range of compositions and synthesis conditions. However, many of the more powerful characterization methods are limited by speed, cost, availability, and/or resolution. To make efficient use of these methods, there is value in developing approaches for identifying critical compositions and conditions to be used as a-priori knowledge for follow-up characterization with high-precision techniques, such as micron-scale synchrotron based X-ray diffraction (XRD). Here we demonstrate the use of optical microscopy and reflectance spectroscopy to identify likely phase-change boundaries in thin film libraries. These methods are used to delineate possible metastable phase boundaries following lateral-gradient Laser Spike Annealing (lg-LSA) of oxide materials. The set of boundaries are then compared with definitive determinations of structural transformations obtained using high-resolution XRD. We demonstrate that the optical methods detect more than 95% of the structural transformations in a composition-gradient La-Mn-O library and a Ga$_2$O$_3$ sample, both subject to an extensive set of lg-LSA anneals. Our results provide quantitative support for the value of optically-detected transformations as a priori data to guide subsequent structural characterization, ultimately accelerating and enhancing the efficient implementation of $mu$m-resolution XRD experiments.
Using resonant X-ray spectroscopies combined with density functional calculations, we find an asymmetric bi-axial strain-induced $d$-orbital response in ultra-thin films of the correlated metal LaNiO$_3$ which are not accessible in the bulk. The sign of the misfit strain governs the stability of an octahedral breathing distortion, which, in turn, produces an emergent charge-ordered ground state with an altered ligand-hole density and bond covalency. Control of this new mechanism opens a pathway to rational orbital engineering, providing a platform for artificially designed Mott materials.
The dielectric function of heteroepitaxial YBiO$_3$ grown on $a$-Al$_2$O$_3$ single crystals via pulsed laser deposition is determined in the spectral range from 0.03 eV to 4.5 eV by simultaneous modeling of spectroscopic ellipsometry and optical transmission data of YBiO$_3$ films of different thickness. The (111)-oriented YBiO$_3$ films are nominally unstrained and crystallize in a defective fluorite-type structure with $Fmbar{3}m$ space group. From the calculated absorption spectrum, a direct electronic bandgap energy of 3.6(1) eV and the signature of an indirect electronic transition around 0.5 eV are obtained. These values provide necessary experimental feedback to previous conflicting electronic band structure calculations predicting either a topologically trivial or non-trivial insulating ground state in YBiO$_3$.
Pulsed laser deposition, a non-equilibrium thin-film growth technique, was used to stabilize metastable tetragonal iron sulfide (FeS), the bulk state of which is known as a superconductor with a critical temperature of 4 K. Comprehensive experiments revealed four important factors to stabilize tetragonal FeS epitaxial thin films: (i) an optimum growth temperature of 300 {deg}C followed by thermal quenching, (ii) an optimum growth rate of ~7 nm/min, (iii) use of a high-purity bulk target, and (iv) use of a single-crystal substrate with small in-plane lattice mismatch (CaF2). Electrical resistivity measurements indicated that none of all the films exhibited superconductivity. Although an electric double-layer transistor structure was fabricated using the tetragonal FeS epitaxial film as a channel layer to achieve high-density carrier doping, no phase transition was observed. Possible reasons for the lack of superconductivity include lattice strain, off-stoichiometry of the film, electrochemical etching by the ionic liquid under gate bias, and surface degradation during device fabrication.
The integration of ferromagnetic and ferroelectric materials into hybrid heterostructures yields multifunctional systems with improved or novel functionality. We here report on the structural, electronic and magnetic properties of the ferromagnetic double perovskite Sr2CrReO6, grown as epitaxial thin film onto ferroelectric BaTiO3. As a function of temperature, the crystal-structure of BaTiO3 undergoes phase transitions, which induce qualitative changes in the magnetic anisotropy of the ferromagnet. We observe abrupt changes in the coercive field of up to 1.2T along with resistance changes of up to 6.5%. These results are attributed to the high sensitivity of the double perovskites to mechanical deformation.
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