Self-assembly of nanostructures with ordered arrangement on the step edges of a vicinal silicon surface has attracted substantial attention 1 and has been demonstrated in several systems, including Au atomic chains, Si atomic wires, periodic clusters, and SiC nanodots arrays. 2 These nanostructures grown using templates of sharp silicon step edges with uniform and controllable size are of potential applications in single-electron transistors, ultra-highdensity storage media, and bionanosensors. 3 In this Communication, we report that pure carbon deposited on a vicinal Si(111)-7×7 surface can assemble into a nanodot array along the sharp step edges with a size ranging from 5 to 30 nm. These nanodots perform a metallic transport on the p-type silicon.We carried out the assembly of carbon nanodots on vicinal silicon surfaces in an ultra-high-vacuum (UHV) apparatus with a base pressure of 10 -10 Torr. The p-type Si(111) substrates with resistivity of ∼0.01 Ωcm were used for deposition. The vicinal silicon (111) surface with sharp and parallel step edges was first reported by the Himpsel group. 4 We prepared the substrate by flashing at 1260°C for 10 s. We quenched it to 800°C in a few seconds to skip the coexisting phase between the 1 × 1 and the 7 × 7 reconstructions around 860°C. Then, the substrate was annealed at 800°C for 10 h with dc current in the direction parallel to the step edge to produce the straight-step array. A pure graphite rod (purity 99.99%) was used as the source of electron-beam evaporation, the deposition rate was controlled at ∼0.04 monolayer (ML)/min (1 ML ) 7.8 × 10 14 atoms/cm 2 ), and the substrate temperature was held around 600°C. The original silicon(111) reconstruction surface and carbon deposited surfaces were observed by Omicron scanning tunneling microscopy (STM) in the UHV apparatus at constant current mode at sample biases between -2 and 2 V and a tunneling current of 0.20-0.25 nA. All STM images were recorded at room temperature. The carbon deposited sample was examined by ultraviolet (UV) micro-Raman to identify bonding structures of carbon nanodots on the silicon surface. Raman spectra were taken by a Renishaw microprobe RM1000B with a 514-nm Ar ion laser at a laser power of 1-2 mW, with light polarized linearly along the step-edge direction. Figure 1a shows the STM image of the Si(111) surface after carbon deposition for 1 h around 600°C. It can be seen that the carbon atoms accumulate and aggregate into nanodots aligned on the sharp and parallel step edges of the vicinal silicon surface. The nanodots have a size ranging from 5 to 30 nm and a height ranging from 0.8 to 3.5 nm and the density is ∼200 µm -2 . The formation of the three-dimensional (3D) nanodots is stimulated by the mismatch between C and Si lattice constants (Volmer-Weber growth mode). 5 From the 3D topographic images shown in Figure 1c, we see that the nanodots exhibit a pyramid-like morphology and clear facets, which means that the nanodots are crystallized. With the increase of deposition time, for example 9...