Abstract
Ferroelectric HfO(2)-based films incorporated in nonvolatile memory devices offer a low-energy, high-speed alternative to conventional memory systems. Oxygen vacancies have been rigorously cited in literature to be pivotal in stabilizing the polar noncentrosymmetric phase responsible for ferroelectricity in HfO(2)-based films. Thus, the ability to regulate and control oxygen vacancy migration in operando in such materials would potentially offer step changing new functionalities, tunable electrical properties, and enhanced device lifespan. Herein, a novel in- operando approach to control both wake-up and fatigue device dynamics is reported. Via clever design of short ad hoc square electrical pulses, both wake-up can be sped up and both fatigue and leakage inside the film can be reduced, key factors for enhancing the performance of memory devices. Using plasmon-enhanced photoluminescence and dark-field spectroscopy (sensitive to <1% vacancy variation), evidence that the electrical pulses give rise to oxygen vacancy redistribution is provided and it is shown that pulse engineering effectively delays wake-up and reduces fatigue characteristics of the HfO(2)-based films. Comprehensive analysis also includes impedance spectroscopy measurements, which exclude any influence of polarization reversal or domain wall movement in interpretation of results.