Multi-ion-beam reactive sputter deposition of ferroelectric Pb(Zr,Ti)O3 thin films

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Abstract
A multi‐ion‐beam reactive sputter (MIBERS) deposition technique was devised to grow ferroelectric lead zirconate titanate (PZT) thin films of different compositions (Zr/Ti ratios of 50/50 and 56/44) from individual metal targets of Pb, Zr, and Ti. This technique offers a highly controllable deposition process allowing excellent uniformity in composition and thickness over a large area (7.5 cm diameter) on a reproducible basis. The PZT films were deposited on a variety of unheated substrates and annealed by two different techniques, rapid thermal annealing and conventional furnace annealing. Both techniques induced a perovskite phase with good morphology. The effect of the excess Pb content was observed in terms of the crystallization and morphology. It was seen that the presence of excess Pb tends to enhance perovskite phase formation but degrades the morphology. The effect of the substrates was observed in terms of crystallization and orientation. A low‐energy oxygen ion beam was employed to modify the film growth. Secondary‐ion bombardment seems to be a promising approach to optimize the film quality as it showed a variety of effects such as enhancing crystallization, inducing preferred orientation, and improving the film morphology. The present MIBERS‐grown PZT films showed fairly high dielectric constants, about 850 for PZT (50/50) and about 1150 for PZT (56/44), and low dielectric losses. Ferroelectricity of these films was established with the values of the remnant polarization and the coercive field for PZT (50/50) of 23 μC/cm2 and 80 kV/cm and for PZT (56/44) of 20 μC/cm2 and 60 kV/cm, respectively. The low‐energy oxygen ion‐beam bombardment during the growth of PZT (50/50) films caused an increase in the dielectric constant to about 1000, reduction in the dissipation factor to 0.02, increase in the remnant polarization to about 26 μC/cm2, and decrease in the coercive field to about 60 kV/cm. The C‐V characteristics of PZT (50/50) films in a metal‐ferroelectric‐metal configuration also indicated a clear dielectric polarization hysteresis.