Dielectric behaviors of Pb1-3x/2LaxTiO3 derived from mechanical activation

To investigate the origin of ultrahigh relative permittivity that has been observed for lanthanum-doped lead titanate, Pb1-3x/2LaxTiO3 (PLT-A) with x ranging from 0.10 to 0.25 were synthesized by mechanical activation of constituent oxides. Their sintered density, grain size and relative permittivity demonstrated a steady increase with increasing of La doping. Upon thermal annealing in oxygen, the relative permittivity of Pb0.70La0.2TiO3 (PLT-A20) at Tc showed an initial rise and a peak at 4h of annealing, and then a steady fall with further increase in annealing time. In contrast, when annealed in nitrogen for 4 h, a significant rise in relative permittivity was observed, although the increase rate falls with prolonged annealing. The observed dependence of relative permittivity and dielectric loss for PLT-A20 on the initial annealing in both oxygen and nitrogen demonstrated the domination of space charge polarization as a result of PbO loss through evaporation from the surface region. While the high activation energy for Pb2+ and O2- diffusion through the surface scale slows down the rate of PbO loss through evaporation, excess loss of PbO adversely affect space charge polarization, leading to a fall in relative permittivity of PLT-A20, upon prolonged annealing in oxygen. In addition to PbO loss, prolonged annealing in nitrogen generated oxygen vacancies, which played an important role in affecting the relative permittivity