Composition-property relationships in high-κ LaxZr1-xOy thin films from aqueous solution

Miniaturization of microelectronic devices has reached a fundamental scaling limit; parasitic electron tunneling through the ultrathin gate dielectric has become a major obstacle to continued device performance. One method for overcoming this limitation is to replace SiO₂ gate dielectrics with thicker high-κ metal oxides. La₂O₃ and ZrO₂ are two such materials that have received significant interest, but low stability to post-anneal water absorption and low-crystallization temperatures, respectively, have limited their widespread use. We recently reported an aqueous, all-inorganic route to high-κ lanthanum zirconium oxide dielectric films (1/1 La/Zr), which mitigates the disadvantages of the binary oxides but maintains their high-κ properties. In this contribution, we vary the La/Zr ratio of the aqueous precursor to optimize the properties of the resulting films. We find that the La_0.20Zr_0.80O_y composition is optimal for providing a high dielectric constant (∼18.2 at 600 °C) while maintaining excellent film morphology and stability. 20% La was necessary to prevent crystallization up to 600 °C, but films with higher La content displayed diminished dielectric constants and decreased stability towards post-anneal water absorption.