Low Temperature Preparation of High-Quality Pb(Zr,Ti)O3 Films by Metal Organic Chemical Vapor Deposition with High Reproducibility

Pb(Zr,Ti)O3 (PZT) is one of the most promising materials for ferroelectric random access memory (FeRAM) application. Among the various preparation methods, metalorganic chemical vapor deposition (MOCVD) has been recognized as a most important one to realize high density FeRAM because of its potential of high-step-coverage and large-area-uniformity of the film quality.In the present study, pulsed-MOCVD was developed in which a mixture of the source gases was pulsed introduced into reaction chamber with interval. By using this deposition technique, simultaneous improvements of the crystallinity, surface smoothness, and electrical property of the film have been reached by comparing to the conventional continuous gas-supplied MOCVD. Moreover, this film had larger remanent polarization (Pr) and lower leakage current density. This is owing to reevaporation of excess Pb element from the film and increase of migration on the surface of substrate during the interval time.This process is also very effective to decrease the deposition temperature of the film having high quality. In fact, the Pr and the leakage current density of polycrystalline Pb(Zr0.35Ti0.65)O3 film deposited at 415 °C were 41.4 μC/cm2 and on the order of 10−7 A/cm2 at 200 kV/cm. This Pr value was almost the same as that of the epitaxially grown film deposited at 415 °C with the same composition corrected for the orientation difference. This suggests that the polycrystalline PZT film prepared by pulsed-MOCVD had the epitaxial-grade ferroelectric properties even through the deposition temperature was as low as 415 °C. Moreover, large “process window” comparable to the process window at 580 °C, above 150 °C higher temperature and was widely used condition, was achieved even at 395°C by the optimization of the deposition condition.