There is significant interest in synthesizing large-area graphene films at low temperatures by chemical vapor deposition (CVD) for nanoelectronic and flexible device applications. However, to date, low-temperature CVD methods have suffered from lower surface coverage because micro-sized graphene flakes are produced. Here, we demonstrate a modified CVD technique for the production of large-area, continuous monolayer graphene films from benzene on Cu at 100–300 °C at ambient pressure. In this method, we extended the graphene growth step in the absence of residual oxidizing species by introducing pumping and purging cycles prior to growth. This led to continuous monolayer graphene films with full surface coverage and excellent quality, which were comparable to those achieved with high-temperature CVD; for example, the surface coverage, transmittance and carrier mobilities of the graphene grown at 300 °C were 100%, 97.6% and 1,900–2,500 cm² V⁻¹ s⁻¹, respectively. In addition, the growth temperature was substantially reduced to as low as 100 °C, which is the lowest temperature reported to date for pristine graphene produced by CVD. Our modified CVD method is expected to allow the direct growth of graphene in device manufacturing processes for practical applications while keeping underlying devices intact.

Controllable and reversible modulation of the electrical and optical properties of WS₂ was demonstrated via hydrazine doping and sulfur annealing.