Growth of ultrahigh density single-walled carbon nanotube forests by improved catalyst design.

We have grown vertically aligned single-walled carbon nanotube forests with an area density of 1.5 × 10(13) cm(-2), the highest yet achieved, by reducing the average diameter of the nanotubes. We use a nanolaminate Fe-Al(2)O(3) catalyst design consisting of three layers of Al(2)O(3), Fe, and Al(2)O(3), in which the lower Al(2)O(3) layer is densified by an oxygen plasma treatment to increase its diffusion barrier properties, to allow a thinner catalyst layer to be used. This high nanotube density is desirable for using carbon nanotubes as interconnects in integrated circuits.

Growth window and possible mechanism of millimeter-thick single-walled carbon nanotube forests.

Our group recently reproduced the water-assisted growth method, so-called "SuperGrowth", of millimeter-thick single-walled carbon nanotube (SWNT) forests by using C2H4/H2/H2O/Ar reactant gas and Fe/Al2O3, catalyst. In this current work, a parametric study was carried out on both reaction and catalyst conditions. Results revealed that a thin Fe catalyst layer (about 0.5 nm) yielded rapid growth of SWNTs only when supported on Al2O3, and that Al2O3 support enhanced the activity of Fe, Co, and Ni catalysts. The growth window for the rapid SWNT growth was narrow, however. Optimum amount of added H2O increased the SWNT growth rate but further addition of H2O degraded both the SWNT growth rate and quality. Addition of H2 was also essential for rapid SWNT growth, but again, further addition decreased both the SWNT growth rate and quality. Because Al2O3 catalyzes hydrocarbon reforming, Al2O3 support possibly enhances the SWNT growth rate by supplying the carbon source to the catalyst nanoparticles. The origin of the narrow window for rapid SWNT growth is also discussed.

A simple combinatorial method aiding research on single-walled carbon nanotube growth on substrates

Establishing fabrication methods of carbon nanotubes (CNTs) is essential to realize many applications expected for CNTs. Catalytic growth of CNTs on substrates by chemical vapor deposition (CVD) is promising for direct fabrication of CNT devices, and catalyst nanoparticles play a crucial role in such growth. We have developed a simple method called "combinatorial masked deposition (CMD)", in which catalyst particles of a given series of sizes and compositions are formed on a single substrate by annealing gradient catalyst layers formed by sputtering through a mask. CMD enables preparation of hundreds of catalysts on a wafer, growth of single-walled CNTs (SWCNTs), and evaluation of SWCNT diameter distributions by automated Raman mapping in a single day. CMD helps determinations of the CVD and catalyst windows realizing millimeter-tall SWCNT forest growth in 10 min, and of growth curves for a series of catalysts in a single measurement when combined with realtime monitoring. A catalyst library prepared using CMD yields various CNTs, ranging from individuals, networks, spikes, and to forests of both SWCNTs and multi-walled CNTs, and thus can be used to efficiently evaluate self-organized CNT field emitters, for example. The CMD method is simple yet effective for research of CNT growth methods. © 2010 The Japan Society of Applied Physics.