Abstract

Defects in two-dimensional and layered materials have attracted interest for realizing properties different from those of perfect crystals. Even stronger links between defect formation, fast growth, and emerging functionality can be found in nanostructures of van der Waals crystals, but only a few prevalent morphologies and defect-controlled synthesis processes have been identified. Here, we show that in vapor–liquid–solid growth of 1D van der Waals nanostructures, the catalyst controls the selection of the predominant (fast-growing) morphologies. Growth of layered GeS over Bi catalysts leads to two coexisting nanostructure types: chiral nanowires carrying axial screw dislocations and bicrystal nanoribbons where a central twin plane facilitates rapid growth. While Au catalysts produce exclusively dislocated nanowires, their modification with an additive triggers a switch to twinned bicrystal ribbons. Nanoscale spectroscopy shows that, while supporting fast growth, the twin defects in the distinctive layered bicrystals are electronically benign and free of nonradiative recombination centers.