Reconfigurable Manipulation of Oxygen Content on Metal Oxide Surfaces and Applications to Gas Sensing.

Oxygen vacancies and adsorbed oxygen species on metal oxide surfaces play important roles in various fields. However, existing methods for manipulating surface oxygen require severe settings and are ineffective for repetitive manipulation. We present a method to manipulate the amount of surface oxygen by modifying the oxygen adsorption energy by electrically controlling the electron concentration of the metal oxide. The surface oxygen control ability of the method is verified using first-principles calculations based on density functional theory (DFT), X-ray photoelectron spectroscopy (XPS), and electrical resistance analysis. The presented method is implemented by fabricating oxide thin film transistors with embedded microheaters. The method can reconfigure the oxygen vacancies on the In2O3, SnO2, and IGZO surfaces so that specific chemisorption dominates. The method can selectively increase oxidizing (e.g., NO and NO) and reducing gas (e.g., H2S, NH3, and CO) reactions by electrically controlling the metal oxide surface to be oxygen vacancy-rich or adsorbed oxygen species-rich. The proposed method is applied to gas sensors and overcomes their existing limitations. The method makes the sensor insensitive to one gas (e.g., H2S) in mixed-gas environments (e.g., NO2+H2S) and provides a linear response (R2 = 0.998) to the target gas (e.g., NO2) concentration within 3 s. We believe that the proposed method is applicable to applications utilizing metal oxide surfaces.