Defect-Induced Phase Transition in Hafnium Oxide Thin Films: Comparing Heavy Ion Irradiation and Oxygen-Engineering Effects

Abstract

Hafnium oxide acts as a functional dielectric in a variety of traditional and emerging nonvolatile memory technologies. To investigate the effect of heavy ion irradiation on its crystalline structure, highly textured hafnium oxide films were irradiated with 1.635 GeV Au ions of fluences ranging from 1\times 10^{9} to 7\times 10^{12} ions/cm2. For monoclinic hafnium oxide films, a fluence-dependent defect-induced phase transition to a defect-stabilized tetragonal phase is identified. In low-temperature tetragonal hafnium oxide films, the X-ray diffraction (XRD) patterns show an out-of-plane lattice constant decrease with increasing irradiation fluence. Observed crystalline changes are strikingly similar to trends found for oxygen-engineered hafnium oxide films, directly grown at varying oxidation conditions. The correlation of structural changes with in vacuo electron spectroscopy data of oxygen-engineered films suggests that the irradiation of hafnium oxide leads to an oxygen loss that increases with fluence. Therefore, the underlying mechanism of the monoclinic to tetragonal phase transition is obviously directly related to oxygen defects. This new information allows predictions of device stability under swift heavy ion irradiation of hafnium oxide-based devices.