Near room temperature chemical vapor deposition of graphene with diluted methane and molten gallium catalyst

Direct growth of graphene integrated into electronic devices is highly desirable but difficult due to the nominal ~1000 °C chemical vapor deposition (CVD) temperature, which can seriously deteriorate the substrates. Here we report a great reduction of graphene CVD temperature, down to 50 °C on sapphire and 100 °C on polycarbonate, by using dilute methane as the source and molten gallium (Ga) as catalysts. The very low temperature graphene synthesis is made possible by carbon attachment to the island edges of pre-existing graphene nuclei islands, and causes no damages to the substrates. A key benefit of using molten Ga catalyst is the enhanced methane absorption in Ga at lower temperatures; this leads to a surprisingly low apparent reaction barrier of ~0.16 eV below 300 °C. The faster growth kinetics due to a low reaction barrier and a demonstrated low-temperature graphene nuclei transfer protocol can facilitate practical direct graphene synthesis on many kinds of substrates down to 50–100 °C. Our results represent a significant progress in reducing graphene synthesis temperature and understanding its mechanism.