Tuning the Optoelectronic Properties of Pulsed Laser Deposited “3D”‐MoS2 Films via the Degree of Vertical Alignment of Their Constituting Layers

Pulsed‐laser‐deposition (PLD) is used to deposit MoS2 thin films at substrate temperatures (Td) ranging from 25 to 700 °C. A Td = 500 °C is identified as the optimal temperature that yields MoS2 films consisting of highly‐crystallized 2H‐MoS2 phase with a strong (002) preferential orientation, a direct optical bandgap (Eg) of ∼1.4 eV and a strong photoresponse of ∼1500%. Raman spectroscopy revealed that the degree of vertical alignment of MoS2 layers in the films also reaches its maximum at Td = 500 °C. High‐resolution‐transmission‐electron‐microscopy has provided a clear‐cut evidence that the PLD‐MoS2 films predominantly consist of vertically aligned MoS2 layers over all the film thickness of ∼90 nm, enabling those “3D” films to behave as a direct‐bandgap “2D‐MoS2” with exceptional optoelectronic properties. Indeed, at Td = 500 °C, the PLD‐MoS2 based photodetectors (PDs) devices are shown to exhibit the highest responsivity (R) and detectivity (D*) values (125 mA W−1 and 9.2 × 109 Jones, respectively) ever reported for large area (≥ 1 cm2) MoS2‐based PDs operating at a voltage as low as 1 V. For the first time, a constant‐plus‐linear relationship between Eg, R, and D* of the PDs and the degree of vertical alignment of the MoS2 layers is established. Such a correlation is fundamental for the controlled growth of PLD‐MoS2 films and the tuning of their properties in view of their integration with standard large‐scale‐integration processing. Pulsed‐laser‐deposition (PLD) is successfully used to deposit vertically‐layered “3D”‐MoS2 films (90 nm‐thick) behaving as a direct‐bandgap “2D‐MoS2” with exceptional structural and optoelectronic properties, particularly at the optimal deposition temperature of 500 °C. The PLD‐MOS2‐based photodetectors exhibit a strong photoresponse of 1500%. Moreover, a linear correlation is established between responsivity and detectivity of the photodetectors and the degree of vertical alignment of the MoS2 layers in the film.