Abstract

Despite widespread interest in the phase-change applications of vanadium dioxide (VO2), the fabrication of high-quality VO2 thin films with elevated transition temperatures (TIMT) and high insulator–metal-transition resistance switching still remains a challenge. This study introduces a two-step atmospheric oxidation approach to fabricate bilayer VO2−x/VO2 films on a c-plane sapphire substrate. To quantify the impact of the VO2 buffer layer, a single-layer VO2 film of the same thickness was also fabricated. The bilayer VO2−x/VO2 films, wherein the top VO2−x film was under-oxidized, demonstrated an elevation in TIMT reaching ∼97 °C, one of the highest reported to date for VO2 films and is achieved in a doping-free manner. Our results also reveal a one-order increase in resistance switching, with the optimum bilayer VO2/VO2 film exhibiting ∼3.6 orders of switching from 25 to 110 °C, compared to the optimum single-layer VO2 reference film. This is accompanied by a one-order decrease in the on-state resistance in its metallic phase. The elevation in TIMT, coupled with increased strain extracted from the XRD characterization of the bilayer film, suggests the possibility of compressive strain along the c-axis. These VO2−x/VO2 films also demonstrate a significant change in the slope of their resistance vs temperature curves contrary to the conventional smooth transition. This feature was ascribed to the rutile/monoclinic quasi-heterostructure formed due to the top VO2−x film having a reduced TIMT. Our findings carry significant implications for both the lucid fabrication of VO2 thin film devices as well as the study of phase transitions in correlated oxides.

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