Composition Dependence of Ferroelectric and Piezoelectric Properties in Lead-Free Ba(Zr0.2Ti0.8)O3-x(Ba0.7Ca0.3)TiO3 Epitaxial Thin Films Prepared by Pulsed Laser Deposition 1School Q.R. Lin1, R. Ding1, B.C. Luo1, D.Y. Wang1,a of Material Science and Engineering, The University of New South Wales, Kensington, NSW 2052, Australia e: dy.wang@unsw.edu.au (1-x) BaZr0.2Ti0.8O3-xBa0.7Ca0.3TiO3 (BZT-xBCT) has been identified as a promising lead-free piezoelectric material due to its high piezoelectric coefficients in bulk form at room temperature morphotropic phase boundary (MPB) composition (x=0.5). However, studies on physical properties of BZT-xBCT thin films are still insufficient. In this work, BZT-xBCT thin films with x = 0.3 - 0.7 were deposited on SrRuO3 electroded SrTiO3 (001) single crystal substrates by pulsed laser deposition. X-ray diffraction and high resolution transmission electron microscope confirmed a highly epitaxial growth of all the films. Both structural and electrical properties demonstrated strong dependence on composition. The optimal ferroelectric and piezoelectric responses were attained in the BZT-0.5BCT thin films with a remanent polarization Pr = 17.8 μC/cm2 and a piezoelectric coefficient d33=100±5 pm/V, indicating an MPB-like behaviour. It should be noted that the observed piezoelectric coefficient of our BZT-0.5BCT thin film is comparable to that of PZT thin films, suggesting the BZT-xBCT thin films are promising lead-free alternative for high performance microelectronic and energy harvesting applications.