Many potential applications of carbon nanotubes are expected to benefit from the availability of single-walled carbon nanotube materials enriched in metallic species, and specifically armchair nanotubes. The present work focuses on the modification of the pulsed laser vaporization (PLV) technique to selectively produce certain carbon nanotube structures. Nanotube nuclei were “warmed-up” with an additional laser pulse, timed to coincide approximately with the nucleation event. The effect of the second laser on the carbon vapor temperature was studied by emission spectroscopy. Nanotube type populations with and without warm-up were compared by means of absorption, photoluminescence, and Raman spectroscopy. It was found that the warm-up of nanotube nuclei with a laser pulse has a noticeable, albeit small, effect on the nanotube population. The intensity of spectral features associated with (9,7) nanotube and its large chiral angle neighbors increased, while small chiral angle nanotubes decreased, with exception of the (15,0) tube. This experiment demonstrates that nanotube population during PLV synthesis can be manipulated in a controlled fashion.