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Monolayers of transition metal dichalcogenides (TMDCs) are atomically thindirect-gap semiconductors with potential applications in nanoelectronics,optoelectronics, and electrochemical sensing. Recent theoretical andexperimental efforts suggest that they are ideal systems for exploiting thevalley degrees of freedom of Bloch electrons. For example, Dirac valleypolarization has been demonstrated in mechanically exfoliated monolayer MoS2samples by polarization-resolved photoluminescence, although polarization hasrarely been seen at room temperature. Here we report a new method forsynthesizing high optical quality monolayer MoS2 single crystals up to 25microns in size on a variety of standard insulating substrates (SiO2, sapphireand glass) using a catalyst-free vapor-solid growth mechanism. The technique issimple and reliable, and the optical quality of the crystals is extremely high,as demonstrated by the fact that the valley polarization approaches unity at 30K and persists at 35% even at room temperature, suggesting a virtual absence ofdefects. This will allow greatly improved optoelectronic TMDC monolayer devicesto be fabricated and studied routinely.

Vapor-Solid Growth of High Optical Quality MoS2 Monolayers With Near-Unity Valley Polarization