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Films of Hf 0.5 Z 0.5 O 2  (HZO) contain a network of grain boundaries. In (111) HZO epitaxial films on (001) SrTiO 3 , for instance, twinned orthorhombic (o‐HZO) ferroelectric crystallites coexist with grain boundaries between o‐HZO and a residual paraelectric monoclinic (m‐HZO) phase. These grain boundaries contribute to the resistive switching response in addition to the genuine ferroelectric polarization switching and have detrimental effects on device performance. Here, it is shown that, by using suitable nanometric capping layer deposited on HZO film, a radical improvement of the operation window of the tunnel device can be achieved. Crystalline SrTiO 3  and amorphous AlO  x   are explored as capping layers. It is observed that these layers conformally coat the HZO surface and allow to increase the yield and homogeneity of ferroelectric junctions while strengthening endurance. Data show that the capping layers block ionic‐like transport channels across grain boundaries. It is suggested that they act as oxygen suppliers to the oxygen‐getters grain boundaries in HZO. In this scenario it could be envisaged that these and other oxides could also be explored and tested for fully compatible CMOS technologies.

Blocking of Conducting Channels Widens Window for Ferroelectric Resistive Switching in Interface‐Engineered Hf 0.5 Zr 0.5 O 2 Tunnel Devices