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[Display omitted] • We achieved ultrathin epitaxial ZnO thin-film actuators on flexible Hastelloy tapes. • We discovered higher piezoelectric constants in thinner epitaxial ZnO thin films. • We demonstrated tunable linear piezoelectric properties in strained ZnO thin films. Linear piezoelectric materials and devices potentially serve as high-accuracy and fast-response sensors and actuators. However, linear piezoelectrics have been scarcely studied, while tuning the linear piezoelectric response of undoped ZnO remains a challenge. Here, linear piezoelectric zinc oxide (ZnO) thin film actuators are fabricated with a sandwich structure of AZO/ZnO/AZO epitaxially on CeO 2 /Hastelloy substrates, with AZO denoting the aluminum-doped ZnO electrodes and CeO 2 denoting the cerium oxide buffer. Due to the lattice mismatch between ZnO and CeO 2 , compressive in-plane lattice strains are detected. Through varying the ZnO layer thickness, a strong correlation is found between the in-plane epitaxial strain and the piezoelectric constant which proves an effective method to improve the linear piezoelectric response of ZnO. Further, the better linear piezoelectric response of the thinner flexible ZnO layer resolves the controversy between the performance and the deformation-durability of flexible piezoelectric ZnO devices. The vertical piezoelectric constant of the ultrathin (∼32 nm) ZnO film is ∼ 8.14 pm/V, which is highly suitable for positioners working at the picometer scale. Future works harnessing the epitaxial strains to further improve the piezoelectric constant of ZnO materials potentially lead to the prosperity of linear piezoelectrics. [ABSTRACT FROM AUTHOR]

[Display omitted] • We achieved ultrathin flexible AZO electrodes with low resistivities (less than100 μΩ•cm). • We demonstrated the mechanical robustness of ultrathin flexible AZO electrodes. • We discovered abnormally high carrier concentrations in strained epitaxial AZO. Aluminum-doped zinc oxide (AZO) thin films are popular transparent electrodes for optoelectronics and photovoltaics. However, next generation flexible devices demand not only high conductivities but also low thicknesses in AZO electrodes to stay robust against deformations. The two requirements contradict each other due to the scattering of carriers at grain boundaries in polycrystalline AZO electrodes. Herein, this work develops ultrathin, highly conductive, single-crystalline, and mechanically robust AZO electrodes on flexible Hastelloy substrates. The epitaxial growth of AZO on polycrystalline Hastelloy is empowered by an advanced buffer architecture topped with a biaxially-textured MgO layer. Thereby, a c -axis epitaxial strain is generated in the AZO electrodes and then regulated by varying the thickness of the electrodes. Abnormally high carrier concentrations are detected in the AZO electrodes likely caused by the piezopotential generated by the epitaxial strain. While the highest resistivity value of the epitaxial AZO electrodes is within the mainstream values of AZO electrodes on various substrates, a resistivity as low as ~22 μΩ•cm is demonstrated in the ultrathin electrode with a thickness of ~28 nm. The mechanical durability of the ultrathin AZO electrode is validated by bending tests of 1000 cycles. [ABSTRACT FROM AUTHOR]

[Display omitted] • We achieved epitaxial linear-piezoelectric ZnO films on flexible substrates. • We enhanced the linear-piezoelectric constant of ZnO with epitaxial strains. • We proved the trivial impacts of textures on the piezoelectric constant of ZnO. Ferroelectrics are popular for sensors, actuators and transducers. However, the energy barrier for reversing the polarization leads to extra energy losses, while the hysteresis causes phase-lags and non-linearities between input and output signals. The high piezoelectric constants of ferroelectrics dictate the figure-of-merit of piezoelectric devices. Enhancing the piezoelectric constant of linear-piezoelectrics potentially leads to next-generation piezoelectric devices free from issues associated with ferroelectrics. By epitaxial growth of undoped ZnO films on flexible Hastelloy substrates, we demonstrated an ~85% improvement in the piezoelectric constant, and more importantly maintained the linearity of the piezoelectric response. Strong out-of-plane and in-plane crystallographic alignments are detected in the epitaxial sample, yet modeling of the effective thin-film piezoelectric constant shows only a limited contribution of the optimized textures. The improvement in the piezoelectric response is ascribed mostly to the in-plane epitaxial strain resulted from the lattice mismatch of ZnO to the substrate. The epitaxial ZnO film on Hastelloy promisingly offer high-precision positioners with nano-/pico-meter resolutions. Enhancing the piezoelectric constant by strain engineering potentially removes the barrier for applications of linear-piezoelectrics and enriches the piezoelectric research community. [ABSTRACT FROM AUTHOR]