Selective electrochemical reactivity of rutile VO2 towards the suppression of metal-insulator transition

We demonstrate through electrolyte gating measurements of a single nanobeam that the rultile phase of VO2 is electrochemically more reactive than the monoclinic phase. Our results show that the complete suppression of the metal-insulator transition and stabilization of the metallic phase is possible when gate voltage is applied in the rutile metallic phase. The results are discussed based on the formation of oxygen vacancies wherein accommodation of a high concentration of vacancies in the rutile phase selectively stabilizes it by disrupting dimerization of adjacent V-V pairs required for a transition to the monoclinic phase. The creation of oxygen vacancies is proposed to proceed through the oxidation of the electrolyte. Raman spectroscopy data suggest surface metallization upon electrolyte gating with an initial coexistence of insulating monoclinic and metallic domains. The selective electrochemical reactivity of the rutile phase and the resulting defect-induced stabilization of this phase across a vastly expanded temperature window suggest a facile defect engineering route to tune electronic phase transitions.