Pyramidal Au20 clusters are intactly deposited and visualized at the single cluster level.

Layered metal monochalcogenides have attracted significant interest in the 2D family since they show different unique properties from their bulk counterparts. The comprehensive synthesis, characterization, and optoelectrical applications of 2D‐layered tin monosulfide (SnS) grown by pulsed laser deposition are reported. Few‐layer SnS‐based field‐effect transistors (FETs) and photodetectors are fabricated on Si/SiO2 substrates. The premium 2D SnS FETs yield an on/off ratio of 3.41 × 106, a subthreshold swing of 180 mV dec−1, and a field effect mobility (µFE) of 1.48 cm2 V−1 s−1 in a 14‐monolayer SnS device. The layered SnS photodetectors show a broad photoresponse from ultraviolet to near‐infrared (365–820 nm). In addition, the SnS phototransistors present an improved detectivity of 9.78 × 1010 cm2 Hz1/2 W−1 and rapid response constants of 60 ms for grow‐time constant τg and 10 ms for decay‐time constant τd under extremely weak 365 nm illumination. This study sheds light on layer‐dependent optoelectronic properties of 2D SnS that promise to be important in next‐generation 2D optoelectronic devices.

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