Sculpting carbon bonds for allotropic transformation through solid-state re-engineering of -sp2 carbon

Carbon forms one of nature's strongest chemical bonds; its allotropes having provided some of the most exciting scientific discoveries in recent times. The possibility of inter-allotropic transformations/hybridization of carbon is hence a topic of immense fundamental and technological interest. Such modifications usually require extreme conditions (high temperature, pressure and/or high-energy irradiations), and are usually not well controlled. Here we demonstrate inter-allotropic transformations/hybridizations of specific types that appear uniformly across large-area carbon networks, using moderate alternating voltage pulses. By controlling the pulse magnitude, small-diameter single-walled carbon nanotubes can be transformed predominantly into larger-diameter single-walled carbon nanotubes, multi-walled carbon nanotubes of different morphologies, multi-layered graphene nanoribbons or structures with sp(3) bonds. This re-engineering of carbon bonds evolves via a coalescence-induced reconfiguration of sp(2) hybridization, terminates with negligible introduction of defects and demonstrates remarkable reproducibility. This reflects a potential step forward for large-scale engineering of nanocarbon allotropes and their junctions.