Isolated-Oxygen-Vacancy Hardening in Lead-Free Piezoelectrics

Defect engineering is a well-established approach to customize the functionalities of perovskite oxides. In demanding high-power applications of piezoelectric materials, acceptor doping serves as the state-of-the-art hardening approach, but inevitably deteriorates the electromechanical properties. Here, a new hardening effect associated with isolated oxygen vacancies for achieving well-balanced performances is proposed. Guided by theoretical design, a well-balanced performance of mechanical quality factor (Q_m) and piezoelectric coefficient (d₃₃) is achieved in lead-free potassium sodium niobate ceramics, where Q_m increases by over 60% while d₃₃ remains almost unchanged. By atomic-scale Z-contrast imaging, hysteresis measurement, and quantitative piezoresponse force microscopy analysis, it is revealed that the improved Q_m results from the inhibition of both extrinsic and intrinsic losses while the unchanged d₃₃ is associated with the polarization contributions being retained. More encouragingly, the hardening effect shows exceptional stability with increasing vibration velocity, offering potential in material design for practical high-power applications such as pharmaceutical extraction and ultrasonic osteotomes.