Layer-Dependent Properties of Ultrathin GeS Nanosheets and Application in UV-Vis Photodetectors

Two-dimensional germanium sulfide (GeS), an analogue of phosphorene, has attracted broad attention owing to its excellent environmental stabilities, fascinating electronic and optical properties, and applications in various nanodevices. In spite of the current achievements on 2D GeS, the report of ultrathin few-layer GeS nanosheets within 5 nm is still lacking. Here in this contribution, we have achieved preparation of ultrathin few-layer GeS nanosheets with thicknesses of 1.3 ± 0.1 nm [approximately three layers (∼3L)], 3.2 ± 0.2 nm (∼6L), and 4.2 ± 0.3 nm (∼8L) via a typical liquid-phase exfoliation (LPE) method. Based on various experimental characterizations and first-principles calculations, the layer-dependent electronic, transport, and optical properties are investigated. For the few-layer GeS nanosheets, enhanced light absorption in the UV-vis region and superior photoresponse behavior with increasing layer number is observed, while for the thin films above 10 nm, the properties degenerate to the bulk feature. In addition, the as-prepared ultrathin nanosheets manifest great potential in the applications of photoelectrochemical (PEC)-type photodetectors, exhibiting excellent and stable periodic photoresponse behavior under the radiation of white light. The ∼8L GeS-based photodetector exhibits superior performance than the thinner GeS nanosheets (<4 nm), even better as compared to the bulk or film (above 10 nm) counterparts in terms of higher photoresponsivity along with remarkable photodetection performance in the UV-vis region. This work not only provides direct and solid evidence of the layer-number evolutionary band structure, mobility, and optical properties of ultrathin 2D GeS nanosheets but also promotes the foreseeable applications of 2D GeS as energy-related photoelectric devices.