Investigation of ferroelectric phase transition for modified barium titanate in multilayer ceramic capacitors by in situ Raman scattering and dielectric measurement

The ferroelectric phase behaviors of modified BaTiO₃ in X7R multilayer ceramic capacitors (MLCCs) were investigated by dielectric measurements and in situ Raman scattering. The in situ thermo-Raman scattering shows that because of a residual stress existing in the MLCCs, the tetragonal to cubic phase transition for modified BaTiO₃ in MLCCs takes place over a wide temperature range of 373 K to 473 K, suggesting a diffuse-like characteristic which can be well explained by a modified phenomenological thermodynamic model, while the dielectric measurement indicates that the tetragonal to cubic transition occurs at 393 K. A disagreement exists between the two experimental results. Furthermore, a dc field-induced paraelectric to ferroelectric transition was identified by the two measurement techniques, but their phase-transition mechanisms are different. The dielectric measurement reveals the polar-micro-region to macro-domain transformation in the shell part of the core–shell structure while the in situ Raman scattering shows the cubic to tetragonal transition under a dc bias field. PACS 74.20.De; 77.22.Ch; 77.84.Dy; 77.80.Bh; 78.30.-j