Abstract
Oxygen vacancies (VO), a common type of point defect in metal oxides materials, play important roles in the physical and chemical properties. To obtain stoichiometric oxide crystal, the pre-existing VO is always removed via careful post-annealing treatment at high temperature in an air or oxygen atmosphere. However, the annealing conditions are difficult to control, and the removal of VO in the bulk phase is restrained because of the high energy barrier of VO migration. Here, we selected VO2 crystal film as the model system and developed an alternative annealing treatment aided by controllable hydrogen doping, which can realize effective removal of VO defects in the VO2-δ crystal at a lower temperature. This finding is attributed to the hydrogenation accelerated oxygen vacancies recovery in the VO2-δ crystal. Theoretical calculations revealed that the H-doping-induced electrons are prone to accumulate around the oxygen defects in the VO2-δ film, which facilitates the diffusion of VO and thus makes it easier to be removed. The methodology is expected to be applied to other metal oxides for oxygen-related point defects control.
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