The armchair carbon nanotube is an ideal system to study fundamental physics in one-dimensional metals and potentially a superb material for applications such as electrical power transmission. Synthesis and purification efforts to date have failed to produce a homogeneous population of such a material. Here we report evolutionary strategies to find DNA sequences for the recognition and subsequent purification of (6,6) and (7,7) armchair species from synthetic mixtures. The new sequences were derived by single-point scanning mutation and sequence motif variation of previously identified ones for semiconducting tubes. Optical absorption spectroscopy of the purified armchair tubes revealed well-resolved first- and second-order electronic transitions accompanied by prominent sideband features that have neither been predicted nor observed previously. Resonance Raman spectroscopy showed a single Lorentzian peak for the in-plane carbon-carbon stretching mode (G band) of the armchair tubes, repudiating the common practice of using such a line shape to infer the absence of metallic species. Our work demonstrates the exquisite sensitivity of DNA to nanotube metallicity and makes the long-anticipated pure armchair tubes available as seeds for their mass amplification.