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We here report the substitution effects of the smaller Ca for the bulky Ba in(Ba1-xCax)(Ti1-yZry)O3 perovskite oxides for two systems (Ba1-xCax)TiO3 withy=0 and (Ba1-xCax)(Ti0.9Zr0.1)O3 with y=0.1. Ca off-centering was found to playa critical role in stabilizing the ferroelectric phase and tuning thepolarization states in both systems. It was demonstrated that the atomicdisplacement due to Ca off-centering in the bulky Ba-site in the perovskitestructure provides an effective approach to compensate the reduction offerroelectricity due to the chemical pressure, which allows to keep the Curiepoint nearly constant in the (Ba1-xCax)TiO3 system and increase the Curie pointin the (Ba1-xCax)(Ti0.9Zr0.1)O3 system. It was commonly observed that the Caoff-centering effects lead to the shift of the R-O and O-T phase transitionstoward lower temperatures and the ferroelectric stability of the T-phase,resulting in the occurrence of quantum phase transitions with interestingphysics phenomena at low temperatures in the (Ba1-xCax)TiO3 system and thegreat enhancement of electromechanical coupling effects around room temperaturein the (Ba1-xCax)(Ti0.9Zr0.1)O3 system over a wide composition range of theCa-concentration. These finding may be of great interest for the design of thegreen piezoelectric materials.

Role of Ca off-centering in tuning the ferroelectric phase transitions in Ba(Zr,Ti)O3 system