Dynamical origins of weakly coupled relaxor behavior in Sn-doped (Ba,Ca)TiO3−BiScO3

Abstract

The peculiar characteristics of relaxors, viz., a frequency-dependent dielectric permittivity peak and good functional properties (dielectric, electromechanical, electrocaloric, etc.), are attributed to nanoscale regions with correlated dipoles, or polar nanoregions (PNRs). However, the exact nature of PNRs and their contribution to relaxor behavior remains debatable. In recent years, solid solutions of $\mathrm{BaTi}{\mathrm{O}}_{3}\text{\ensuremath{-}}\mathrm{Bi}\mathrm{Me}{\mathrm{O}}_{3}$ (where Me is a metal), have emerged as an interesting system with characteristics in between that of relaxors and dipole glasses. Here, we have examined the atomistic origins of weakly coupled relaxor behavior, specifically with regard to formation of PNRs, in Sn-doped $(1\ensuremath{-}x)(\mathrm{Ba},\mathrm{Ca})\mathrm{Ti}{\mathrm{O}}_{3}\text{\ensuremath{-}}x\mathrm{BiSc}{\mathrm{O}}_{3}$ using macroscopic polarization and neutron dynamic pair distribution function measurements. We show that the short-range atomic correlations observed within the PNRs dynamically fluctuate with frequencies of the order of THz. Furthermore the composition-dependent dielectric and polarization behaviors are critically influenced by the relative stability of the atomic correlations near \ensuremath{\sim}1 THz, while the instantaneous atomic correlations are largely independent of $x$. The current results are discussed based on a model of intrinsic local modes distributed in a dielectrically soft matrix.