Journal
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
Volume 91, Issue 11, Pages 3690-3697Publisher
WILEY
DOI: 10.1111/j.1551-2916.2008.02708.x
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Funding
- United States Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]
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The high permittivity of Pb(Zr,Ti)O-3 and (Pb,La)(Zr,Ti)O-3-PZT and PLZT, respectively-thin films and the flexibility of chemical solution deposition (CSD) make solution-derived P(L)ZT thin films extremely attractive for integrated capacitor applications. However, Pb-loss or cation segregation during processing results in degraded properties of the final film. Here, we have extended the use of multivariate statistical analysis (MSA) of energy-dispersive spectroscopy (EDS) spectrum images (SIs) in scanning transmission electron microscopy (STEM) to allow the two-dimensional (2D) quantitative analysis of cation segregation and depletion in P(L)ZT thin films. Quantified STEM-EDS SIs allow high-resolution (< approximate to 10 nm) quantification of these cation distributions. Surface Pb depletion is found after crystallization and is replenished by a unique post-crystallization PbO overcoat+anneal processes. Zr/Ti and La segregation are found to develop in a decidedly nonplanar fashion during crystallization, especially in PLZT 12/70/30 material, highlighting the need for 2D analysis. Quantitative 2D chemical information is essential for improved processing of homogeneous P(L)ZT films with optimal electrical properties.
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