The nucleation and growth kinetics of single-wall carbon nanotubes in aligned arrays have been measured using fast pulses of acetylene and in situ optical diagnostics in conjunction with low pressure chemical vapor deposition (CVD). Increasing the acetylene partial pressure is shown to decrease nucleation times by three orders of magnitude, permitting aligned nanotube arrays to nucleate and grow to micrometers lengths within single gas pulses at high (up to 7 μm/s) peak growth rates and short ∼0.5 s times. Low-frequency Raman scattering (>10 cm(-1)) and transmission electron microscopy measurements show that increasing the feedstock flux in both continuous- and pulsed-CVD shifts the product distribution to large single-wall carbon nanotube diameters >2.5 nm. Sufficiently high acetylene partial pressures in pulsed-CVD appear to temporarily terminate the growth of the fastest-growing, small-diameter nanotubes by overcoating the more catalytically active, smaller catalyst nanoparticles within the ensemble with non-nanotube carbon in agreement with a growth model. The results indicate that subsets of catalyst nanoparticle ensembles nucleate, grow, and terminate growth within different flux ranges according to their catalytic activity.