Rapid growth and flow-mediated nucleation of millimeter-scale aligned carbon nanotube structures from a thin-film catalyst.

We discuss the rapid growth of films and lithographically templated microstructures of vertically aligned small-diameter multiwalled carbon nanotubes (VA-MWNTs), by atmospheric-pressure thermal chemical vapor deposition (CVD) of C2H4/H2/Ar on a Fe/Al2O3 catalyst film deposited by electron beam evaporation. The structures grow to 1 mm height in 15 min and reach close to 2 mm in 60 min. The growth rate and final height of CNT microstructures grown from catalyst patterns depend strongly on the local areal density of catalyst, representing a reverse analogue of loading effects which occur in plasma etching processes. Abrupt transitions between areas of micrometer-thick tangled CNT films and millimeter-scale aligned CNT structures are manipulated by changing the duration of pretreatment by H2/Ar prior to introduction of C2H4 and by changing the configuration of the substrate sample in the furnace tube. This demonstrates that the flow profile over the sample mediates the supply of reactants to the catalyst and that pretreatment using H2 significantly affects the initial activity of the catalyst.