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We report on the growth of single-walled carbon nanotubes from a monometallic Co catalyst on an oxidized Si wafer support by the most simple growth recipe (vacuum annealing, growth by undiluted C2H2). Nevertheless,
multiwavelength Raman spectroscopy and transmission electron spectroscopy show a remarkable selectivity for chiral indices and thus, e.g., high abundance with a single chirality representing 58% of all semiconducting tubes. In situ x-ray photoelectron spectroscopy monitors the catalyst chemistry during carbon nanotube growth and shows interfacial Co-Si interactions that may help to stabilize the nanoparticle/nanotube diameter. We outline a two-mechanism model explaining the selective growth.