Critical Insight into Pretransitional Behavior and Dielectric Tunability of Relaxor Ceramics

Materials (Basel). 2023 Dec 13;16(24):7634. doi: 10.3390/ma16247634.

Abstract

This model discussion focuses on links between the unique properties of relaxor ceramics and the basics of Critical Phenomena Physics and Glass Transition Physics. It indicates the significance of uniaxiality for the appearance of mean-field type features near the paraelectric-to-ferroelectric phase transition. Pretransitional fluctuations, that are increasing up to the size of a grain and leading to inter-grain, random, local electric fields are responsible for relaxor ceramics characteristics. Their impact yields the pseudospinodal behavior associated with "weakly discontinuous" local phase transitions. The emerging model redefines the meaning of the Burns temperature and polar nanoregions (PNRs). It offers a coherent explanation of "dielectric constant" changes with the "diffused maximum" near the paraelectric-to-ferroelectric transition, the sensitivity to moderate electric fields (tunability), and the "glassy" dynamics. These considerations are challenged by the experimental results of complex dielectric permittivity studies in a Ba0.65Sr0.35TiO3 relaxor ceramic, covering ca. 250 K, from the paraelectric to the "deep" ferroelectric phase. The distortion-sensitive and derivative-based analysis in the paraelectric phase and the surrounding paraelectric-to-ferroelectric transition reveal a preference for the exponential scaling pattern for ε(T) changes. This may suggest that Griffith-phase behavior is associated with mean-field criticality disturbed by random local impacts. The preference for the universalistic "critical & activated" evolution of the primary relaxation time is shown for dynamics. The discussion is supplemented by a coupled energy loss analysis. The electric field-related tunability studies lead to scaling relationships describing their temperature changes.

Keywords: critical phenomena; dielectric properties; glassy dynamics; modeling; relaxor ceramics.