There are many potential applications of ferroelectric thin films that take advantage of their unique dielectric and piezoelectric properties, such as tunable microwave devices and thin-film active sensors for structural health monitoring (SHM). However, many technical issues still restrict practical applications of ferroelectric thin films, including high insertion loss, limited figure of merit, soft mode effect, large temperature coefficients, and others. The main theme of this thesis is the advanced technique developments, and the new ferroelectric thin films syntheses and investigations for novel device applications.

A novel method of additional doping has been adopted to (Ba,Sr)TiO ₃ (BSTO) thin films on MgO. By introducing 2% Mn into the stoichiometric BSTO, Mn:BSTO thin films have shown a greatly enhanced dielectric tunability and a reduced insertion loss at high frequencies (10-30 GHz). A new record of a large tunability of 80% with a high dielectric constant of 3800 and an extra low dielectric loss of 0.001 at 1 MHz at room-temperature was achieved. Meanwhile, the new highly epitaxial ferroelectric (Pb,Sr)TiO₃ (PSTO) thin films have been synthesized on (001) MgO substrates. PSTO films demonstrated excellent high frequency dielectric properties with high dielectric constants above 1420 and large dielectric tunabilities above 34% at room-temperature up to 20 GHz. In addition, a smaller temperature coefficient from 80 K to 300 K was observed in PSTO films compared to BSTO films. These results indicate that the Mn:BSTO and PSTO films are both good candidates for developing room-temperature tunable microwave devices.

Furthermore, crystalline ferroelectric BaTiO₃ (BTO) thin films have been deposited directly on metal substrate Ni through a unique in-situ substrate pre-oxidation treatment. The highly oriented nanopillar structural BTO films were grown on the buffered layers created by the pre-oxidation treatment. No interdiffusion or reaction was observed at the interface. As-grown BTO films demonstrated good ferroelectric properties and an extremely large piezoelectric response of 130 (x 10^-12 C/N). These excellent preliminary results enable the long-term perspective on the unobtrusive ferroelectric thin-film active sensors for SHM applications.