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Large Magnetic Susceptibility Anisotropy of Metallic Carbon Nanotubes

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 Added by Junichiro Kono
 Publication date 2010
  fields Physics
and research's language is English




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Through magnetic linear dichroism spectroscopy, the magnetic susceptibility anisotropy of metallic single-walled carbon nanotubes has been extracted and found to be 2-4 times greater than values for semiconducting single-walled carbon nanotubes. This large anisotropy is consistent with our calculations and can be understood in terms of large orbital paramagnetism of electrons in metallic nanotubes arising from the Aharonov-Bohm-phase-induced gap opening in a parallel field. We also compare our values with previous work for semiconducting nanotubes, which confirm a break from the prediction that the magnetic susceptibility anisotropy increases linearly with the diameter.

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We study theoretically the impact of Zener tunneling on the charge-transport properties of quasi-metallic (Qm) carbon nanotubes (characterized by forbidden band gaps of few tens of meV). We also analyze the interplay between Zener tunneling and elastic scattering on defects. To this purpose we use a model based on the master equation for the density matrix, that takes into account the inter-band Zener transitions induced by the electric field (a quantum mechanical effect), the electron-defect scattering and the electron-phonon scattering. In presence of Zener tunnelling the Qm tubes support an electrical current even when the Fermi energy lies in the forbidden band gap. In absence of elastic scattering (in high quality samples), the small size of the band gap of Qm tubes enables Zener tunnelling for realistic values of the the electric field (above $sim$ 1 V/mu m). The presence of a strong elastic scattering (in low quality samples) further decreases the values of the field required to observe Zener tunnelling. Indeed, for elastic-scattering lengths of the order of 50 nm, Zener tunnelling affects the current/voltage characteristic already in the linear regime. In other words, in quasi-metallic tubes, Zener tunneling is made more visible by defects.
The quantum corrections to the frequencies of the $Gamma$ point longitudinal optical (LO) and transverse optical (TO) phonon modes in carbon nanotubes are investigated theoretically. The frequency shift and broadening of the TO phonon mode strongly depend on the curvature effect due to a special electron-phonon coupling in carbon nanotubes, which is shown by the Fermi energy dependence of the frequency shift for different nanotube chiralities. It is also shown that the TO mode near the $Gamma$ point decouples from electrons due to local gauge symmetry and that a phonon mixing between LO and TO modes is absent due to time-reversal symmetry. Some comparison between theory and experiment is presented.
A phonon frequency shift of the radial breathing mode for metallic single wall carbon nanotubes is predicted as a function of Fermi energy. Armchair nanotubes do not show any frequency shift while zigzag nanotubes exhibit phonon softening, but this softening is not associated with the broadening. This chirality dependence originates from a curvature-induced energy gap and a special electron-phonon coupling mechanism for radial breathing modes. Because of the particle-hole symmetry, only the off-site deformation potential contributes to the frequency shift. On the other hand, the on-site potential contributes to the Raman intensity, and the radial breathing mode intensity is stronger than that of the $G$ band. The relationship between the chirality dependence of the frequency shift of the radial breathing mode and the $Gamma$ point optical phonon frequency shift is discussed.
We report the observation of the intrinsic magnetic susceptibility of highly purified SWCNT samples prepared by a combination of acid treatment and density gradient ultracentrifugation (DGU). We observed that the diamagnetic susceptibility of SWCNTs increases linearly with increasing nanotube diameter. We found that the magnetic susceptibility divided by the diameter is a universal function of the scaled temperature. Furthermore, the estimated magnetic susceptibilities of pure semiconducting and pure metallic SWCNT samples suggest that they respond differently to changes in carrier density, which is consistent with theory. These findings provide experimental verification of the theoretically predicted diameter, temperature, and metallicity dependence of the magnetic susceptibility.
We have calculated the effects of structural distortions of armchair carbon nanotubes on their electrical transport properties. We found that the bending of the nanotubes decreases their transmission function in certain energy ranges and leads to an increased electrical resistance. Electronic structure calculations show that these energy ranges contain localized states with significant $sigma$-$pi$ hybridization resulting from the increased curvature produced by bending. Our calculations of the contact resistance show that the large contact resistances observed for SWNTs are likely due to the weak coupling of the NT to the metal in side bonded NT-metal configurations.
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