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Ferroelectric Bi2SiO5 (BSO) thin films were deposited by pulsed laser deposition on Nb-doped (100), (110) and (111) SrTiO3 (Nb:STO) substrates, resulting in (001)-, (113)- and (204)-oriented epitaxial films. Due to the crystallinity of BSO, in which the Bi2O2 layers are formed perpendicular to the c-axis direction, the (001)-oriented epitaxial BSO thin film showed the lowest remanent polarization and the best leakage current characteristics. On the other hand, the (113)- and (204)-oriented films showed an increase in remanent polarization due to the improvement of a-oriented crystallinity. Through experiments using vertical and lateral piezoresponse force microscopy, it has been confirmed that the distribution of in-plane-oriented domains reducing remanent polarization decreases in the order of (001)-, (113)- and (204)-oriented epitaxial BSO thin films. The epitaxial BSO thin films that exhibit ferroelectric hysteresis loops similar to the relaxor ferroelectric thin films tended to have improved energy storage characteristics as a result of improved remanent polarization and saturation polarization. In particular, the (113)-oriented epitaxial BSO thin film showed a high recoverable energy density of about 41.6 J cm−3 and an energy storage efficiency of about 85.6%.

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