Composition gradient optimization and electrical characterization of (Pb, Ca)TiO3 thin films

Compositionally graded (Pb, Ca)TiO3 thin films were prepared by a monoethanolamine-modified sol–gel technique on platinum-coated silicon substrates at the annealing temperature of 600 °C. The composition gradient of the films was greatly improved by a modified annealing method. The dielectric constants, for up-graded and down-graded films annealed at 600 °C for 60 min, were found to be 469 and 355, respectively. Both were larger than those reported for conventional (Pb, Ca)TiO3 thin films. The compositionally graded films had large polarization offsets in hysteresis loops when excited by an alternating electric field. The more smooth the composition gradient of the graded film, the larger the polarization offset. This was consistent with a theoretical model reported previously by Mantese and coworkers [Appl. Phys. Lett. 71, 2047 (1997)]. The magnitude of polarization offset displayed a power-law dependence on the electric field, and the direction of the offset depended on the direction of the composition gradient with respect to the substrate. Both up-graded and down-graded films had good leakage current characteristics.