Systems with a ferroelectric to paraelectric transition in the vicinity of room temperature are useful for devices. Adjusting the ferroelectric transition temperature (T(c)) is traditionally accomplished by chemical substitution-as in Ba(x)Sr(1-x)TiO(3), the material widely investigated for microwave devices in which the dielectric constant (epsilon(r)) at GHz frequencies is tuned by applying a quasi-static electric field. Heterogeneity associated with chemical substitution in such films, however, can broaden this phase transition by hundreds of degrees, which is detrimental to tunability and microwave device performance. An alternative way to adjust T(c) in ferroelectric films is strain. Here we show that epitaxial strain from a newly developed substrate can be harnessed to increase T(c) by hundreds of degrees and produce room-temperature ferroelectricity in strontium titanate, a material that is not normally ferroelectric at any temperature. This strain-induced enhancement in T(c) is the largest ever reported. Spatially resolved images of the local polarization state reveal a uniformity that far exceeds films tailored by chemical substitution. The high epsilon(r) at room temperature in these films (nearly 7,000 at 10 GHz) and its sharp dependence on electric field are promising for device applications.
A strong correlation is observed between the structure and the microwave dielectric properties of epitaxial Ba0.5Sr0.5TiO3 (BST) thin films deposited onto (001) MgO by pulsed laser deposition. Films were deposited at 750 °C in an oxygen pressure that was varied from 3 to 1000 mTorr. The tetragonal distortion (ratio of in-plane and surface normal lattice parameters, D=a/c) of the films depends on the oxygen deposition pressure. D varied from 0.996 at 3 mTorr to 1.003 at 800 mTorr. At microwave frequencies (1–20 GHz), BST films with low distortion have higher dielectric constants (ε∼500), and lower dielectric loss (tan δ∼0.02) compared to films with higher distortion. The correlation of the microwave properties with the film structure can be attributed to stresses and polarizability in the film. The BST film grown at the oxygen deposition pressure of 50 mTorr exhibits a large dielectric constant change and a low dielectric loss at the same time, which corresponds to the film in low stress (D=1.0004). For tunable microwave applications, BST films with low stress are desirable in order to achieve both low dielectric loss and large tunability.
The dielectric properties of Ba0.6Sr0.4TiO3 (BST) and 1.0, 20.0, 40.0, and 60.0 wt % MgO-mixed BST bulk ceramics and thin films were investigated for tunable microwave applications. The effects of MgO mixing with BST on BST phase transitions were examined. It is observed that Mg substitution into BST causes a shift in the cubic-tetragonal BST phase transition peak to a lower temperature. Mg-substituted BST and MgO-mixed phases exhibit depressed and broadened BST phase transition peaks, resulting in decreased dielectric constants and dielectric losses at room temperature. BST and 1.0, 20.0, 40.0, and 60.0 wt % MgO-mixed BST thin films (∼0.3 μm thick) were deposited on (100) MgO single-crystal substrates at 750°C in an oxygen ambient pressure of 200 mTorr by pulsed laser deposition. The MgO–BST composite thin films showed a relatively high dielectric Q (=1/tan δ) compared to the pure BST and Mg-substituted BST thin films while retaining useful dielectric tuning.
Oriented, single phase thin films (∼5000 Å thick) of Ba0.5Sr0.5TiO3 (BST) have been deposited onto (100) MgO and (100) LaAlO3 (LAO) substrates using pulsed laser deposition. The capacitance and dielectric Q (1/tan δ) of as-deposited and annealed films have been measured from 1 to 20 GHz as a function of electric field (0–80 kV/cm) at room temperature using interdigitated Ag electrodes deposited on top of the film. For films deposited onto MgO, it is observed that, after a postdeposition anneal (1000–1200 °C), the dielectric constant decreases and the dielectric Q increases. For films deposited onto LAO, a postdeposition anneal (⩽ 1000 °C) resulted in a significant increase in the dielectric constant and a decrease in Q. The observed dielectric properties of the BST films are attributed to the changes in film stress, which affects the extent of ionic polarization.
Epitaxial Ba1−xSrxTiO3 (BST) thin films have been deposited onto (100)MgO and LaAlO3 substrates using pulsed-laser deposition. Thick (>1 μm) Ag interdigitated capacitors capped with a thin protective layer of Au have been deposited on top of the BST films using electron-beam deposition. The capacitance (C) and dielectric quality factor (Q=1/tan δ) of the structure has been measured at microwave frequencies (1–20 GHz) as a function of electric field (E⩽67 kV/cm) at room temperature. In epitaxial BST films, either high dielectric tuning (4:1), which is defined as {[C(0)−C(E)]/C(0)}×100, or high dielectric Q (∼100–250) was observed but not both at the same time. Film strain was observed by x-ray diffraction and is closely related to the dielectric properties as limiting the ability to obtain both high tuning and high dielectric Q in epitaxial BST thin films. A thin BST buffer layer was used to relieve the strain in the films. In strain-relieved films, both dielectric tuning and dielectric Q were increased after annealing. A theoretical analysis of the strain effect of the films is presented based on Devonshire thermodynamic theory.
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