Layer-by-layer thinning of MoSe2 by soft and reactive plasma etching

Two-dimensional (2D) transition metal dichalcogenides (TMDs) like molybdenum diselenide (MoSe2) have recently gained considerable interest since their properties are complementary to those of graphene. Unlike gapless graphene, the band structure of MoSe2 can be changed from the indirect band gap to the direct band gap when MoSe2 changed from bulk material to monolayer. This transition from multilayer to monolayer requires atomic-layer-precision thining of thick MoSe2 layers without damaging the remaining layers. Here, we present atomic-layer-precision thinning of MoSe2 nanaosheets down to monolayer by using SF6 + N2 plasmas, which has been demonstrated to be soft, selective and high-throughput. Optical microscopy, atomic force microscopy, Raman and photoluminescence spectra suggest that equal numbers of MoSe2 layers can be removed uniformly regardless of their initial thickness, without affecting the underlying SiO2 substrate and the remaining MoSe2 layers. By adjusting the etching rates we can achieve complete MoSe2 removal and any disired number of MoSe2 layers including monolayer. This soft plasma etching method is highly reliable and compatible with the semiconductor manufacturing processes, thereby holding great promise for various 2D materials and TMD-based devices.