Solvent-Free Preparation of Closely Packed MoS₂ Nanoscrolls for Improved Photosensitivity

Due to their enhanced light absorption efficiency, one-dimensional (1D) transition metal dichalcogenide (TMDC) nanoscrolls derived from two-dimensional (2D) TMDC nanosheets have shown excellent optoelectronic properties. Currently, organic solvent and alkaline droplet-assisted scrolling methods are popular for preparing TMDC nanoscrolls. Unfortunately, the adsorption of organic solvent or alkaline impurities on TMDC is inevitable during the preparation, which affects the optoelectronic properties of TMDC. In this work, we report a solvent-free method to prepare closely packed MoS₂ nanoscrolls by dragging a deionized water droplet onto the chemical vapor deposition grown monolayer MoS₂ nanosheets at 100 °C (referred to as MoS₂ NS-W). The as-prepared MoS₂ NS-W was well characterized by optical microscopy, atomic force microscopy, and ultralow frequency (ULF) Raman spectroscopy. After high temperature annealing, the height of MoS₂ nanoscrolls prepared using an ethanol droplet (referred to as MoS₂ NS-E) greatly decreased, indicating the loss of encapsulated ethanol in MoS₂ NS-E. While the height of MoS₂ NS-W was almost unchanged under the same conditions, implying that no water was embedded in the scroll. Compared to the MoS₂ NS-E, the MoS₂ NS-W shows more ULF breathing mode peaks, confirming the stronger interlayer interaction. In addition, the MoS₂ NS-W shows a higher Young's modulus than MoS₂ NS-E, which could arise from the closely packed scroll structure. Importantly, the MoS₂ NS-W device showed a photosensitivity 1 order of magnitude higher than that of the MoS₂ NS-E device under blue, green, and red lasers, respectively. The decreased photosensitivity of MoS₂ NS-E was attributed to the larger dark current, which might be assigned to the adsorbed ethanol between the adjacent layers in MoS₂ NS-E. Our work provides a solvent-free method to prepare closely packed MoS₂ nanoscrolls at large scale and demonstrates their great potential for high-performance optoelectronic devices.