Evidence for reversible oxygen ion movement during electrical pulsing: enabler of emerging ferroelectricity in binary oxides

Ferroelectric HfO₂-based materials and devices show promising potential for applications in information technology but face challenges with inadequate electrostatic control, degraded reliability, and serious variation in effective oxide thickness scaling. We demonstrate a novel interface-type switching strategy to realize ferroelectric characteristics in atomic-scale amorphous binary oxide films, which are formed in oxygen-deficient conditions by atomic layer deposition at low temperatures. This approach can avoid the shortcomings of reliability degradation and gate leakage increment in scaling polycrystalline doped HfO₂-based films. Using theoretical modeling and experimental characterization, we show the following. (1) Emerging ferroelectricity exists in ultrathin oxide systems as a result of microscopic ion migration during the switching process. (2) These ferroelectric binary oxide films are governed by an interface-limited switching mechanism, which can be attributed to oxygen vacancy migration and surface defects related to electron (de)trapping. (3) Transistors featuring ultrathin amorphous dielectrics, used for non-volatile memory applications with an operating voltage reduced to ±1 V, have also been experimentally demonstrated. These findings suggest that this strategy is a promising approach to realizing next-generation complementary metal-oxide semiconductors with scalable ferroelectric materials.