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Local-gate multilayer MoS2 phototransistors exhibit a photoresponsivity of up to 342.6 A W(-1) , which is higher by 3 orders of magnitude than that of global-gate multilayer MoS2 phototransistors. These simulations indicate that the gate underlap is critical for the enhancement of the photoresponsivity. These results suggest that high photoresponsivity can be achieved in indirect-bandgap multilayer MoS2 phototransistors by optimizing the optoelectronic design.

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.