Synthesis of large-area rhombohedral few-layer graphene by chemical vapor deposition on copper

Rhombohedral-stacked few-layer graphene (FLG) displays peculiar electronic properties that could lead to phenomena such as high-temperature superconductivity and magnetic ordering. To date, experimental studies have been mainly limited by the difficulty in isolating rhombohedral FLG with thickness exceeding 3 layers and device-compatible size. In this work, we demonstrate the synthesis and transfer of rhombohedral graphene with thickness up to 9 layers and areas up to ∼50 μm². The domains of rhombohedral FLG are identified by Raman spectroscopy and are found to alternate with Bernal regions within the same crystal in a stripe-like configuration. Near-field nano-imaging further confirms the structural integrity of the respective stacking orders. Combined spectroscopic and microscopic analyses indicate that rhombohedral-stacking formation is strongly correlated to the underlying copper step-bunching and emerges as a consequence of interlayer displacement along preferential crystallographic orientations. The growth and transfer of rhombohedral FLG with the reported thickness and size shall facilitate the observation of predicted unconventional physics and ultimately add to its technological relevance.