The recently discovered two-dimensional (2D) group IV chalcogenides attract much attention owing to their novel electronic and photonic properties. All the reported materials of this class favor (distorted) octahedral coordination via p bonding; by contrast, in the dichalcogenides where the bonding tendency approaches sp3, no corresponding 2D phase has been realized so far. Here, by engineering the composition of a chalcogenide heterostructure, the hitherto elusive GeTe2 is experimentally observed in a confined 2D environment. Density functional theory simulations predict the existence of a freestanding monolayer of octahedrally coordinated GeTe2 under tensile strain, and the existence of GeSe2 and GeS2 in the same form under equilibrium conditions. These 2D germanium dichalcogenides are either metallic or narrow gap semiconducting, and may lead to new applications in nanoscale electronics.
