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  1. Charge transport mechanisms governing DC resistance degradation in ferroelectric films are influenced by defects, particularly oxygen vacancies. This paper demonstrates that oxygen vacancies migrate in lead zirconate titanate (PZT) films under a DC bias field and contribute to resistance degradation. Model PZT thin films were developed in which the concentration and distribution of oxygen vacancies were controlled via (a) changing the dopant type and concentration from 1%–4% Mn (acceptor) to 1%–4% Nb (donor) or (b) annealing undoped PZT films at varying partial pressures of PbO. The presence of associated (immobile) and dissociated (mobile) oxygen vacancies was distinguished by thermally stimulated depolarization current (TSDC) measurements. The impact of mobile oxygen vacancies on local defect chemistry and associated charge transport mechanisms was explored by electron energy loss spectroscopy (EELS). For Mn-doped PZT films, following resistance degradation, TSDC studies revealed only one depolarization peak with an activation energy of 0.6–0.8 eV; this peak was associated with ionic space charge presumably due to migration of oxygen vacancies. The magnitude of the depolarization current peak increased with increasing degradation times. A similar depolarization current peak attributed to the existence of mobile oxygen vacancies was also observed for undoped and Nb-doped PZT films; the magnitude ofmore »this peak decreased as the Nb or PbO contents in PZT films increased. An additional TSDC peak associated with polaron hopping between Ti3+ and Ti4+ was found in both Nb-doped PZT films and undoped PZT films annealed under low PbO partial pressure. Degraded Nb-doped samples exhibited a chemical shift in the TiL2,3 peak to lower energy losses and the appearance of shoulders on the t2g and eg peaks, implying a reduction of Ti cations in regions near the cathode.« less
  2. Medical ultrasound and other devices that require transducer arrays are difficult to manufacture, particularly for high frequency devices (>30 MHz). To enable focusing and beam steering, it is necessary to reduce the center-to-center element spacing to half of the acoustic wavelength. Conventional methodologies prevent co-sintering ceramic–polymer composites due to the low decomposition temperatures of the polymer. Moreover, for ultrasound transducer arrays exceeding 30 MHz, methods such as dice-and-fill cannot provide the dimensional tolerances required. Other techniques in which the ceramic is formed in the green state often fail to retain the required dimensions without distortion on firing the ceramic. This paper explores the use of the cold sintering process to produce dense lead zirconate titanate (PZT) ceramics for application in high frequency transducer arrays. PZT–polymer 2-2 composites were fabricated by cold sintering tape cast PZT with Pb nitrate as a sintering aid and ZnO as the sacrificial layer. PZT beams of 35 μm width with ~5.4 μm kerfs were produced by this technique. The ZnO sacrificial layer was also found to serve as a liquid phase sintering aid that led to grain growth in adjacent PZT. This composite produced resonance frequencies of >17 MHz.