Interstitial Mo‐Assisted Photovoltaic Effect in Multilayer MoSe2 Phototransistors

Thin‐film transistors (TFTs) based on multilayer molybdenum diselenide (MoSe₂) synthesized by modified atmospheric pressure chemical vapor deposition (APCVD) exhibit outstanding photoresponsivity (103.1 A W^?1), while it is generally believed that optical response of multilayer transition metal dichalcogenides (TMDs) is significantly limited due to their indirect bandgap and inefficient photoexcitation process. Here, the fundamental origin of such a high photoresponsivity in the synthesized multilayer MoSe₂ TFTs is sought. A unique structural characteristic of the APCVD‐grown MoSe₂ is observed, in which interstitial Mo atoms exist between basal planes, unlike usual 2H phase TMDs. Density functional theory calculations and photoinduced transfer characteristics reveal that such interstitial Mo atoms form photoreactive electronic states in the bandgap. Models indicate that huge photoamplification is attributed to trapped holes in subgap states, resulting in a significant photovoltaic effect. In this study, the fundamental origin of high responsivity with synthetic MoSe₂ phototransistors is identified, suggesting a novel route to high‐performance, multifunctional 2D material devices for future wearable sensor applications.     

A highly sensitive chemical gas detecting transistor based on highly crystalline CVD-grown MoSe<Subscript>2</Subscript> films

Layered semiconductors with atomic thicknesses are becoming increasingly important as active elements in high-performance electronic devices owing to their high carrier mobilities,large surface-to-volume ratios,and rapid electrical responses to their surrounding environments.Here,we report the first implementation of a highly sensitive chemical-vapor-deposition-grown multilayer MoSe2 field-effect transistor (FET) in a NO2 gas sensor.This sensor exhibited ultra-high sensitivity (S =ca.1,907 for NO2 at 300 ppm),real-time response,and rapid on-off switching.The high sensitivity of our MoSe2 gas sensor is attributed to changes in the gap states near the valence band induced by the NO2 gas absorbed in the MoSe2,which leads to a significant increase in hole current in the off-state regime.Device modeling and quantum transport simulations revealed that the variation of gap states with NO2 concentration is the key mechanism in a MoSe2 FET-based NO2 gas sensor.This comprehensive study,which addresses material growth,device fabrication,characterization,and device simulations,not only indicates the utility of MoSe2 FETs for high-performance chemical sensors,but also establishes a fundamental understanding of how surface chemistry influences carrier transport in layered semiconductor devices.