ABSTRACT:The colors of suspended metallic colloidal particles are determined by their size-dependent plasma resonance, while those of semiconducting colloidal particles are determined by their size-dependent band gap. Here, we present a novel case for armchair carbon nanotubes, suspended in aqueous medium, for which the color depends on their sizedependent excitonic resonance, even though the individual particles are metallic. We observe distinct colors of a series of armchair-enriched nanotube suspensions, highlighting the unique coloration mechanism of these one-dimensional metals.The size-dependent colors of suspended colloidal particles have fascinated researchers, engineers, and artists for centuries. While quantum confinement always plays a fundamental role, the coloration mechanism can differ depending on whether the particles are metallic or semiconducting. For metallic nanoparticles, their colors are determined by the freecarrier plasma resonance whose frequency depends on the electron density as well as the particle size and shape. 1 For semiconducting nanoparticles, the key parameter is the sizedependent fundamental band gap, i.e., the separation between the top of the valence band (HOMO) and the bottom of the conduction band (LUMO), which sensitively changes with quantum confinement, i.e., size. 2 Here, we present a novel case for armchair single-walled carbon nanotubes (SWCNTs), suspended in aqueous medium, for which the origin of their color depends on the interband excitonic resonance even though the individual particles are gapless, i.e., metallic. Armchair nanotubes enjoy a rather special status among the SWCNT family. The structure of each member, or species, of the family is uniquely specified by a pair of integers, (n,m), resulting in different species possessing different diameters, chiral angles, and electronic types (semiconducting or metallic). 3 Armchair SWCNTs are characterized by the simple relation n = m, i.e., (n,n), and they are known to be the only truly gapless species with excellent electrical properties, exhibiting ballistic conduction even at room temperature. 4 At the same time, their one-dimensional characteristics combined with their linear band dispersions have attracted much fundamental interest for exploring many-body phenomena. 5 However, systematic studies of macroscopic ensembles of armchair nanotubes have been impossible due to the coexistence of different (n,m) species of nanotubes in asgrown samples.Recent years have seen impressive progress in post-growth separation of SWCNTs using a variety of methods. One of the most successful methods has been density gradient ultracentrifugation (DGU), 6-10 which can sort out different species of SWCNTs in bulk quantities according to their diameters, chiralities, and electronic types, enabling studies of (n,m)-dependent properties using standard macroscopic characterization measurements. In a recent report, 10 we provided unambiguous evidence of bulk enrichment of armchair nanotubes through DGU by utilizing wavelength-dependen...