Publications

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Fine powders of calcium zirconate (CaZrO{sub 3}, CZ) and calcium titanate (CaTiO{sub 3}, CT) were synthesized using a nonaqueous oxalate co-precipitation route from Ca(NO{sub 3}){sub 2}{center_dot}4 H{sub 2}O and group(IV) n-butoxides (Ti(OBu{sup n}){sub 4} or Zr(OBu{sup n}){sub 4}). Several reaction conditions and batch sizes (2-35 g) were explored to determine their influence on final particle size, morphology, and phase. Characterization of the as-prepared oxalate precursors, oven dried oxalate precursors (60-90 C), and calcined powders (635-900 C) were analyzed with TGA/DTA, XRD, TEM, and SEM. Densification and sintering studies on pressed CZ pellets at 1375 and 1400 C were also performed. Through the developed oxalate co-precipitation route, densification temperatures for CZ were lowered by 125 C from the 1500 C firing temperature required for conventional mixed oxide powders. Low field electrical tests of the CZ pellets indicated excellent dielectric properties with dielectric constants of {approx}30 and a dissipation factor of 0.0004 were measured at 1 kHz.

This report focuses on our recent advances in the fabrication and processing of barium strontium titanate (BST) thin films by chemical solution depositiion for next generation fuctional integrated capacitors. Projected trends for capacitors include increasing capacitance density, decreasing operating voltages, decreasing dielectric thickness and decreased process cost. Key to all these trends is the strong correlation of film phase evolution and resulting microstructure, it becomes possible to tailor the microstructure for specific applications. This interplay will be discussed in relation to the resulting temperature dependent dielectric response of the BST films.

Lead loss during processing of solution-derived Pb(Zr,Ti)O3 (PZT)-based thin-films can result in the formation of a Pb-deficient, nonferroelectric fluorite phase that is detrimental to dielectric properties. It has recently been shown that this nonferroelectric fluorite phase can be converted to the desired perovskite phase by postcrystallization treatment. Here, quantitative standard-based energy-dispersive x-ray spectrometry (EDS) in a scanning transmission electron microscope (STEM) is used to study cation distribution before and after this fluorite-to-perovskite transformation. Single-phase perovskite PbZr0.53 Ti0.47O3 (PZT 53 /47) and Pb0.88 La0.12 Zr0.68 Ti0.29O3 (PLZT 12/70/30) specimens that underwent this treatment were found to be chemically indistinguishable from the perovskite present in the multiphase specimens prior to the fluorite-to-perovskite transformation. Significant Zr-Ti segregation is found in PLZT 12/70/30, but not in PZT 53/47. Slight La-segregation was seen in rapidly crystallized PLZT, but not in more slowly crystallized PLZT.

The high permittivity of Pb(Zr,Ti)O3 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 (< ≈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. © 2008 Sandia Corporation. Journal compilation © 2008 The American Ceramic Society.

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This report focuses on our recent advances in the fabrication and processing of barium strontium titanate (BST) thin films by chemical solution deposition for next generation functional integrated capacitors. Projected trends for capacitors include increasing capacitance density, decreasing operating voltages, decreasing dielectric thickness and decreased process cost. Key to all these trends is the strong correlation of film phase evolution and resulting microstructure, it becomes possible to tailor the microstructure for specific applications. This interplay will be discussed in relation to the resulting temperature dependent dielectric response of the BST films.

Chemical solution deposition has been used to fabricate continuous ultrathin lead lanthanum zirconate titanate (PLZT) films as thin as 20 nm. Further, multilayer capacitor structures with as many as 10 dielectric layers have been fabricated from these ultrathin PLZT films by alternating spin-coated dielectric layers with sputtered platinum electrodes. Integrating a photolithographically defined wet etch step to the fabrication process enabled the production of functional multilayer stacks with capacitance values exceeding 600 nF. Such ultrathin multilayer capacitors offer tremendous advantages for further miniaturization of integrated passive components.

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A facile solution-based processing route using standard spin-coating deposition techniques has been developed for the production of reliable capacitors based on lead lanthanum zirconate titanate (PLZT) with active areas of ≥1 mm2 and dielectric layer thicknesses down to 50 nm. With careful control of the dielectric phase development through improved processing, ultrathin capacitors exhibited slim ferroelectric hysteresis loops and dielectric constants of >1000, similar to those of much thicker films. Thus, it has been demonstrated that chemical solution deposition is a viable route to the production of capacitor films which are as thin as 50 nm but are still macroscopically addressable with specific capacitance values >160 nF/mm2.

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