We have developed a new method with which we can for the first time produce self-aligned cobalt silicide (CoSi 2 ) nanostructures from Co nanoparticles. These nanostructures are formed by reacting Co nanoparticles with Si substrates at 900°C. Their dimensions are normally 3 to 10 nm wide and up to a few micrometers long. The orientations of these nanostructures are controlled by the crystalline substrate, as they are orthogonally and hexagonally aligned on Si(100) and Si(111), respectively. Because these self-aligned nanostructures (SAN) are thermally stable up to 1000°C in air and chemically inert to prolonged treatment with strong acids, and because their sizes are uniform and much smaller than those made from lithography, they can be ideal materials for making components such as electric contacts, interconnects, and gates for future nanoelectronics.One dimensional crystalline materials such as carbon nanotubes and nanowires made of ZnO, GaN, InP, and Si have been the focus of many studies in the past decade. 1-3 Challenges to the applications of these materials arise not only from making them but also from manipulating them to form devices. It is thus advantageous if one can directly produce desired nanostructures on suitable substrates for device fabrication. Such methods are usually called a bottom-up approach, and the starting materials are often monolayers or sub-monolayers of atoms. 4-7 Lithography, on the other hand, is a top-down method. It relies on the making and breaking of large, uniform materials such as thin films. Thus, if crystalline films are available, lithography can also be used to make microstructures. 8-10 For example, using this top-down method, submicrometer cobalt silicide structures have been made. 10-15 These structures can be used as contacts, gates, and interconnects in microelectronics because cobalt silicides are an excellent conductor and are thermally and chemically stable. However, the dimensions of the structures so fabricated using the top-down approach are much larger than those of the nanotubes and nanowires mentioned above.We report here a new method to directly synthesize as small as sub-5 nm and uniform CoSi 2 self-aligned nanostructures (SAN) with the bottom-up approach. Instead of using layers of atoms, our method uses nanoparticles (NP) of different sizes. The products are silicide crystalline nanostructures aligned on Si wafers. Co nanoparticles were made by following the reported procedure. 16 In brief, 0.54 g of Co 2 (CO) 8 was dissolved in 3-mL of oxygen-free, anhydrous dichlorobenzene in a drybox. The solution was then injected into a mixture of oleic acid, trioctylphosphine oxide, and trioctylamine at a temperature slightly above the boiling point of dichlorobenzene under Ar. After several minutes, portions of the solution were withdrawn from the reaction flask and placed in Ar-filled vials. Depending on the ratios of the surfactants, different sized Co nanoparticles were made, and their sizes were verified by transmission electron microscopy (TEM). Figure 1a sh...