The existence of morphotropic phase boundary (MPB) inside HfO2-ZrO2 solid solution thin films has been predicted; if it exists, it provides up a new path toward an ideal silicon-compatible dielectric....

Engineering of HfO 2 −ZrO 2 ferroelectric thin films can substantially increase their dielectric constant. Here, we investigate dielectric and structural properties of ∼10 nm thin films consisting of stacked 1 nm thin ferroelectric (FE) Hf 1−x Zr x O 2 (HZO(x)) and antiferroelectric (AFE) ZrO 2 layers. At x < 0.5, the measurements of polarization vs electric field revealed pure FE hysteresis loops, whereas at x > 0.5, pinched hysteresis loops with some remnant polarization were observed, which indicate a coexistence of FE and AFE orderings. Finally, a pure ZrO 2 thin film (x = 1) exhibits only an AFE double hysteresis loop. In this way, we demonstrate that the coexistence of FE and AFE orderings can be controlled by adjusting the composition of HZO(x) layers in the HZO(x)/ZrO 2 nanolaminate films. At x = 0.5, the dielectric constant is ∼60 in nanolaminate films, which is much higher than that of the conventional HZO(x) solid solution thin films. Structural investigations confirm a coexistence of polar orthorhombic and nonpolar tetragonal structures, which is consistent with the observed polarization hysteresis loops. We also show that the strain generated in the nanolaminate structure significantly facilitates a field-induced transition from the AFE to the FE phase. The design does not considerably affect the leakage current in HZO(x)/ZrO 2 nanolaminate films, which makes this system highly promising for complementary metal oxide semiconductor-compatible capacitors.

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A large coercive field EC of HfO2 based ferroelectric devices poses critical performance issues in their applications as ferroelectric memories and ferroelectric field effect transistors. A new design to reduce EC by fabricating nanolaminate Hf0.5Zr0.5O2 / ZrO2 (HZZ) thin films is used, followed by an ensuing annealing process at a comparatively high temperature 700 °C. High-resolution electron microscopy imaging detects tetragonal-like domain walls between orthorhombic polar regions. These walls decrease the potential barrier of polarization reversal in HfO2 based films compared to the conventional domain walls with a single non-polar spacer, causing about a 40% decrease in EC. Capacitance vs. electric field measurements on HZZ thin film uncovered a substantial increase of dielectric permittivity near the EC compared to the conventional Hf0.5Zr0.5O2 thin film, justifying the higher mobility of domain walls in the developed HZZ film. The tetragonal-like regions served as grease easing the movement of the domain wall and reducing EC

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