We investigate the electronic structure of a perovskite-type Pauli paramagnet SrMoO3 (t2g 2 ) thin film using hard x-ray photoemission spectroscopy and compare the results to the realistic calculations that combine the density functional theory within the local-density approximation (LDA) with the dynamical-mean field theory (DMFT). Despite the clear signature of electron correlations in the electronic specific heat, the narrowing of the quasiparticle bands is not observed in the photoemission spectrum. This is explained in terms of the characteristic effect of Hund's rule coupling for partiallyfilled t2g bands, which induces strong quasiparticle renormalization already for values of Hubbard interaction which are smaller than the bandwidth. The interpretation is supported by additional model DMFT calculations including Hund's rule coupling, that show renormalization of low-energy quasiparticles without affecting the overall bandwidth. The photoemission spectra show additional spectral weight around −2 eV that is not present in the LDA+DMFT. We interpret this weight as a plasmon satellite, which is supported by measured Mo, Sr and Oxygen core-hole spectra that all show satellites at this energy.
Single-crystalline thin films of CaMoO3 and SrMoO3 with a Mo4+ state perovskite structure have been epitaxially grown by pulsed-laser deposition from Mo6+ state ceramic targets. Phase-pure films were obtained on nearly lattice-matched perovskite substrates using argon gas flow during the deposition. Transport properties of the films are consistent with those of paramagnetic and metallic phases, whereas the residual resistivities are far lower than those reported previously for films and bulk polycrystals. These results indicate that this growth method can be useful for exploring the interfaces and junction properties of 4d and 5d transition metal oxides that are unstable in a conventional oxidative atmosphere.
The optical properties of pulsed laser deposited highly crystalline SrMoO3 thin films were investigated. Due to their low resistivity below 30 μΩ cm, thin films of SrMoO3 are candidates for transparent conductor applications. The transparency of SrMoO3 extends into the ultraviolet range to about 300 nm. In this range, SrMoO3 has a higher transparency at similar sheet resistance as compared to alternative oxide or metallic materials. Density functional theory shows that electron-electron correlation effects are small in SrMoO3 as compared to other low-resistivity transition metal oxides and predicts the optical properties in good agreement with experiment.
In the field of oxide electronics, there has been tremendous progress in the recent years in atomic engineering of functional oxide thin films with controlled interfaces at the unit cell level. However, some relevant devices such as tunable ferroelectric microwave capacitors (varactors) based on BaxSr1−xTiO3 are stymied by the absence of suited compatible, very low resistive oxide electrode materials on the micrometer scale. Therefore, we start with the epitaxial growth of the exceptionally highly conducting isostructural perovskite SrMoO3 having a higher room-temperature conductivity than Pt. In high-frequency applications such as tunable filters and antennas, the desired electrode thickness is determined by the electromagnetic skin depth, which is of the order of several micrometers in the frequency range of a few gigahertz. Here, we report the pulsed laser deposition of a fully layer-by-layer grown epitaxial device stack, combining a several micrometers thick electrode of SrMoO3 with atomically engineered sharp interfaces to the substrate and to the subsequently grown functional dielectric layer. The difficult to achieve epitaxial thick film growth makes use of the extraordinary ability of perovskites to accommodate strain well beyond the critical thickness limit by adjusting their lattice constant with small shifts in the cation ratio, tuned by deposition parameters. We show that our approach, encompassing several orders of magnitude in film thickness scale whilst maintaining atomic layer control, enables the fabrication of metal-insulator-metal (MIM) varactors based on 50–100 nm thin BaxSr1−xTiO3 layers with high tunability above three at the Li-ion battery voltage level (3.7 V).
We have measured the microwave resistance of highly conducting perovskite oxide SrMoO3 thin film coplanar waveguides. The epitaxial SrMoO3 thin films were grown by pulsed laser deposition and showed low mosaicity and smooth surfaces with a root mean square roughness below 0.3 nm. Layer-by-layer growth could be achieved for film thicknesses up to 400 nm as monitored by reflection high-energy electron diffraction and confirmed by X-ray diffraction. We obtained a constant microwave resistivity of 29 μΩ·cm between 0.1 and 20 GHz by refining the frequency dependence of the transmission coefficients. Our result shows that SrMoO3 is a viable candidate as a highly conducting electrode material for all-oxide microwave electronic devices.
We have investigated the origin of superstructure peaks as observed by X-ray diffraction of multiferroic Bi(Fe0.5Cr0.5)O3 thin films grown by pulsed laser deposition on single crystal SrTiO3 substrates. The photon energy dependence of the contrast between the atomic scattering factors of Fe and Cr is used to rule out a chemically ordered double perovskite Bi2FeCrO6 (BFCO). Structural calculations suggest that the experimentally observed superstructure occurs due to unequal cation displacements along the pseudo-cubic [111] direction that mimic the unit cell of the chemically ordered compound. This result helps to clarify discrepancies in the correlations of structural and magnetic order reported for Bi2FeCrO6. The observation of a superstructure in itself is not a sufficient proof of chemical order in double perovskites.
The Ni content of LaNi1−xO3 epitaxial thin films grown by pulsed laser deposition has been varied by ablation from targets with different composition. While tensile strain and Ni substoichiometry reduce the conductivity, nearly stoichiometric and unstrained films show reproducibly resistivities below 100 μΩ × cm. Since the thermodynamic instability of the Ni3+ state drives defect formation, Ni defect engineering is the key to obtain highly conducting LaNiO3 thin films.
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