Tuning the Built-in Electric Field in Ferroelectric Pb(Zr0.2Ti0.8)O3 Films for Long-Term Stability of Single-Digit Nanometer Inverted Domains

The emergence of new technologies, such as whole genome sequencing systems, which generate a large amount of data, is requiring ultrahigh storage capacities. Due to their compactness and low power consumption, probe-based memory devices using Pb(Zr0.2Ti0.8)O3 (PZT) ferroelectric films are the ideal candidate for such applications where portability is desired. To achieve ultrahigh (>1 Tbit/in2) storage densities, sub-10 nm inverted domains are required. However, such domains remain unstable and can invert back to their original polarization due to the effects of an antiparallel built-in electric field in the PZT film, domain-wall, and depolarization energies. Here, we show that the built-in electric-field can be tuned and suppressed by repetitive hydrogen and oxygen plasma treatments. Such treatments trigger reversible Pb reduction/oxidation activity, which alters the electrochemistry of the Pb overlayer and compensates for charges induced by the Pb vacancies. This tuning mechanism is used to demonstrate the writing of stable and equal size sub-4 nm domains in both up- and down-polarized PZT films, corresponding to eight inverted unit-cells. The bit sizes recorded here are the smallest ever achieved, which correspond to potential 60 Tbit/in2 data storage densities.