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The catalytic sites of MoS$_{2}$ monolayers towards hydrogen evolution arewell known to be vacancies and edge-like defects. However, it is still verychallenging to control the position, size, and defective areas on the basalplane of Mo$S_{2}$ monolayers by most of defect-engineering routes. In thiswork, the fabrication of etched arrays on ultra-large supported andfree-standing MoS$_{2}$ monolayers using focused ion beam (FIB) is reported forthe first time. By tuning the Ga+ ion dose, it is possible to confine defectsnear the etched edges or spread them over ultra-large areas on the basal plane.The electrocatalytic activity of the arrays toward hydrogen evolution reaction(HER) was measured by fabricating microelectrodes using a new method thatpreserves the catalytic sites. We demonstrate that the overpotential can bedecreased up to 290 mV by assessing electrochemical activity only at the basalplane. High-resolution transmission electron microscopy images obtained on FIBpatterned freestanding MoS$_{2}$ monolayers reveal the presence of amorphousregions and X-ray photoelectron spectroscopy indicates sulfur excess in theseregions. Density-functional theory calculations provide identification ofcatalytic defect sites. Our results demonstrate a new rational control ofamorphous-crystalline surface boundaries and future insight for defectoptimization in MoS$_{2}$ monolayers.

Patterning edge-like defects and tuning defective areas on the basal plane of ultra-large MoS$_{2}$ monolayers toward hydrogen evolution reaction