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).

Perovskite oxide materials of the general chemical formula ABO3 are a rich playground for epitaxial stacks of different functional layers for novel device applications. In the example of a tunable metal–insulator–metal ferroelectric varactor (tunable capacitor) made from the highest conducting perovskite SrMoO3 as an electrode and the tunable dielectric Ba0.5Sr0.5TiO3 (BST), we show how the extremely conflicting oxidation potentials can be conciliated in a fully functional heterostructure. Controlling the growth kinetics by the substrate temperature, oxygen pressure, and oxidation time, the formation of the non-conducting Mo6+ states can be effectively suppressed and the BST cation stoichiometry can be tuned. The cumulative impact of the cation nonstoichiometry, epitaxial strain, and oxygen deficiency in the BST films leads to the expansion of their c-axis lattice parameter via the formation of point defects. The dielectric permittivity of 440, the high tunability of 3.5, and the quality factor of 50 are achieved for the varactors at the frequency of 1 GHz. It turns out that the varactor performance is anti-correlated to the tetragonal lattice distortion of BST, which itself is interrelated to the oxidation conditions. The mechanism of the leakage current through oxygen deficient BST layers of the varactors is analyzed within the combined scenarios of the space-charge limited current and Poole–Frenkel field-assisted emission from traps. The achieved high capacitance per unit area of 0.04 pF/μm2 and moderate leakage currents of 0.025 μA/pF make these varactors suitable for applications in microwave microelectronic devices.

Transition metal perovskite oxide SrMoO3 with a Mo4+ 4d2 electronic configuration exhibits a room-temperature resistivity of 5.1 μΩcm in a single-crystal form and, therefore, is considered a prominent conducting electrode material for all-oxide microelectronic devices. Stabilization of the unfavorable Mo4+ valence state in SrMoO3 thin films necessitates reductive growth conditions that are often incompatible with a highly oxidative environment necessary to grow epitaxial heterostructures with fully oxygenated functional layers (e.g., tunable dielectric BaxSr1−xTiO3). Interestingly, only a few unit cells of the perovskite titanate capping layers SrTiO3, BaTiO3, and Ba0.5Sr0.5TiO3 act as an efficient oxygen barrier and minimize SrMoO3 oxidation into electrically insulating SrMoO4 in the broad range of the thin-film growth parameters. The Mo valence state in SrMoO3, determined by x-ray photoelectron spectroscopy, is used to analyze oxygen diffusion through the capping layers. The lowest level of oxygen diffusion is observed in Ba0.5Sr0.5TiO3. A Ba0.5Sr0.5TiO3 film with a thickness of only 6 unit cells preserves the Mo4+ oxidation state in the SrMoO3 underlayer up to the oxygen partial pressure of 8 mTorr at the temperature of 630 °C. Results, therefore, indicate that SrMoO3 films covered with atomically thin Ba0.5Sr0.5TiO3 remain conducting in an oxygen environment and can be integrated into all-oxide thin-film heterostructures with other functional materials.

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