▎ 摘　　要

Applying time-dependent photoemission we unravel the graphene growth process on a metallic surface by chemical vapor deposition (CVD). Graphene CVD growth is in stark contrast to the standard growth process of two-dimensional films because it is self-limiting and stops as soon as a monolayer of graphene has been synthesized. Most importantly, a novel phase of metastable graphene was discovered that is characterized by permanent and simultaneous construction and deconstruction. The high quality and large area graphene flakes are characterized by angle-resolved photoemission, proving that they are indeed monolayer and cover the whole 1 x 1 cm Ni(111) substrate. These findings are of high relevance to the intensive search for reliable synthesis methods for large graphene flakes of controlled layer number.