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Direct growth of large-area vertically stacked two-dimensional (2D) van derWaal (vdW) materials is a prerequisite for their high-end applications inintegrated electronics, optoelectronics and photovoltaics. Currently,centimetre- to even metre-scale monolayers of single-crystal graphene (MLG) andhexagonal boron nitride (h-BN) have been achieved by epitaxial growth onvarious single-crystalline substrates. However, in principle, this success inmonolayer epitaxy seems extremely difficult to be replicated to bi- orfew-layer growth, as the full coverage of the first layer was believed toterminate the reactivity of those adopting catalytic metal surfaces. Here, wereport an exceptional layer-by-layer chemical vapour deposition (CVD) growth oflarge size bi-layer graphene single-crystals, enabled by self-transmittingcatalytic activity from platinum (Pt) surfaces to the outermost graphenelayers. In-situ growth and real-time surveillance experiments, underwell-controlled environments, unambiguously verify that the growth does followthe layer-by-layer mode on open surfaces of MLG/Pt(111). First-principlescalculations indicate that the transmittal of catalytic activity is allowed byan appreciable electronic hybridisation between graphene overlayers and Ptsurfaces, enabling catalytic dissociation of hydrocarbons and subsequentlydirect graphitisation of their radicals on the outermost sp2 carbon surface.This self-transmitting catalytic activity is also proven to be robust fortube-furnace CVD in fabricating single-crystalline graphene bi-, tri- andtetra-layers, as well as h-BN few-layers. Our findings offer an exceptionalstrategy for potential controllable, layer-by-layer and wafer-scale growth ofvertically stacked few-layered 2D single crystals.

Layer-by-layer growth of bilayer graphene single-crystals enabled by self-transmitting catalytic activity