Correlation between charge density wave phase transition and hydrogen adsorption in 1T-TaS2 thin film devices

Abstract

Thin films of tantalum disulfide in the 1T-polytype structural phase (1T-TaS2), a type of metallic two-dimensional (2D) transition metal dichalcogenides (TMDs), are reactive to H2. Interestingly, in the incommensurate charge-density wave (ICCDW) phase with a metallic state, the electrical resistance of the 1T-TaS2 thin film decreases when H2 is adsorbed on it and returns to its initial value upon desorption. In contrast, the electrical resistance of the film in the nearly commensurate CDW (NCCDW) phase, which has a subtle band overlap or a small bandgap, does not change upon H2 adsorption/desorption. This difference in H2 reactivity is a result of differences in the electronic structure of the two 1T-TaS2 phases, namely, the ICCDW and NCCDW phases. Compared to other semiconductor 2D-TMDs such as MoS2 and WS2, the metallic TaS2 has been theoretically proven to capture gas molecules more easily because Ta has a stronger positive charge than Mo or W. Our experimental results provide evidence of this. Notably, this study is the first example of H2 sensing using 1T-TaS2 thin films and demonstrates the possibility of controlling the reactivity of the sensors to the gas by changing the electronic structure via CDW phase transitions.