In-situ Observation of Surface Graphitization of Gallium Droplet and Concentration of Carbon in Liquid Gallium

Although carbon has been recognized to be insoluble in gallium, we found that the outermost surface of gallium has unexpectedly high carbon solubility, particularly the limited region of about a few nanometers in depth. Our in-situ transmission electron microscope observations revealed that a graphene layer was precipitated at the surface of a gallium droplet simultaneously with gallium evaporation, and some of the droplets created an internal graphitic layer. On the basis of these experimental data, we evaluated a substantial carbon solubility that seemed to exceed about 50 at. %, but was realized in a very thin surface region of about 4 nm in depth. We believe that this high carbon solubility at the gallium surface is the key mechanism for the catalytic ability of gallium that was observed at the interface between liquid gallium and solid amorphous carbon.