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Register a new userBand structure dependent electronic localization in macroscopic films of single-chirality single-wall carbon nanotubes
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Much understanding exists regarding chirality-dependent properties of single-wall carbon nanotubes (SWCNTs) on a single-tube level. However, macroscopic manifestations of chirality dependence have been limited, especially in electronic transport, despite the fact that such distinct behaviors are needed for any applications of SWCNT-based devices. In addition, developing reliable transport theory is challenging since a description of localization phenomena in an assembly of nanoobjects requires precise knowledge of disorder on multiple spatial scales, particularly if the ensemble is heterogeneous. Here, we report the observation of pronounced chirality-dependent electronic localization in temperature and magnetic field dependent conductivity measurements on single-chirality SWCNT films. The samples included semiconducting (6,5) and (10,3) films, chiral metallic (7,4) and (8,5) films, and armchair (6,6) films. Experimental data and theoretical calculations revealed variable-range-hopping dominated transport in all samples except the armchair SWCNT film. We obtained localization lengths that fall into three distinct categories depending on their band gaps. The clear deviation of the armchair films from the other films suggests their robustness toward defects and possible additional transport mechanisms. Our detailed analyses on electronic transport properties of single-chirality SWCNT films provide significant new insight into electronic transport in ensembles of nanoobjects, offering foundations for designing and deploying macroscopic SWCNT solid-state devices.
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Optical properties of single-wall carbon nanotubes (SWCNTs) for light polarized parallel to the nanotube axis have been extensively studied, whereas their response to light polarized perpendicular to the nanotube axis has not been well explored. Here, by using a macroscopic film of highly aligned single-chirality (6,5) SWCNTs, we performed a systematic polarization-dependent optical absorption spectroscopy study. In addition to the commonly observed angular-momentum-conserving interband absorption of parallel-polarized light, which generates $E_{11}$ and $E_{22}$ excitons, we observed a small but unambiguous absorption peak whose intensity is maximum for perpendicular-polarized light. We attribute this feature to the lowest-energy cross-polarized interband absorption processes that change the angular momentum along the nanotube axis by $pm 1$, generating $E_{12}$ and $E_{21}$ excitons. The energy difference between the $E_{12}$ and $E_{21}$ exciton peaks, expected from asymmetry between the conduction and valence bands, was smaller than the observed linewidth. Unlike previous observations of cross-polarized excitons in polarization-dependent photoluminescence and circular dichroism spectroscopy experiments, our direct observation using absorption spectroscopy allowed us to quantitatively analyze this resonance. Specifically, we determined the energy and oscillator strength of this resonance to be 1.54 and 0.05, respectively, compared with the values for the $E_{11}$ exciton peak. These values, in combination with comparison with theoretical calculations, in turn led to an assessment of the environmental effect on the strength of Coulomb interactions in this aligned single-chirality SWCNT film.
We present a systematic study of the electronic and magnetic properties of transition-metal (TM) atomic chains adsorbed on the zigzag single-wall carbon nanotubes (SWNTs). We considered the adsorption on the external and internal wall of SWNT and examined the effect of the TM coverage and geometry on the binding energy and the spin polarization at the Fermi level. All those adsorbed chains studied have ferromagnetic ground state, but only their specific types and geometries demonstrated high spin polarization near the Fermi level. Their magnetic moment and binding energy in the ground state display interesting variation with the number of $d-$electrons of the TM atom. We also show that specific chains of transition metal atoms adsorbed on a SWNT can lead to semiconducting properties for the minority spin-bands, but semimetallic for the majority spin-bands. Spin-polarization is maintained even when the underlying SWNT is subjected to high radial strain. Spin-dependent electronic structure becomes discretized when TM atoms are adsorbed on finite segments of SWNTs. Once coupled with non-magnetic metal electrodes, these magnetic needles or nanomagnets can perform as spin-dependent resonant tunnelling devices. The electronic and magnetic properties of these nanomagnets can be engineered depending on the type and decoration of adsorbed TM atom as well as the size and symmetry of the tube. Our study is performed by using first-principles pseudopotential plane wave method within spin-polarized Density Functional Method.
We present a simple technique which uses a self-aligned oxide etch to suspend individual single-wall carbon nanotubes between metallic electrodes. This enables one to compare the properties of a particular nanotube before and after suspension, as well as to study transport in suspended tubes. As an example of the utility of the technique, we study quantum dots in suspended tubes, finding that their capacitances are reduced owing to the removal of the dielectric substrate.
Low field and high field transport properties of carbon nanotubes/polymer composites are investigated for different tube fractions. Above the percolation threshold f_c=0.33%, transport is due to hopping of localized charge carriers with a localization length xi=10-30 nm. Coulomb interactions associated with a soft gap Delta_CG=2.5 meV are present at low temperature close to f_c. We argue that it originates from the Coulomb charging energy effect which is partly screened by adjacent bundles. The high field conductivity is described within an electrical heating scheme. All the results suggest that using composites close to the percolation threshold may be a way to access intrinsic properties of the nanotubes by experiments at a macroscopic scale.
The possibility of low-energy surface plasmon amplification by optically excited excitons in small-diameter single wall carbon nanotubes is theoretically demonstrated. The nonradiative exciton-plasmon energy transfer causes the buildup of the macroscopic population numbers of coherent localized surface plasmons associated with high-intensity coherent local fields formed at nanoscale throughout the nanotube surface. These strong local fields can be used in a variety of new optoelectronic applications of carbon nanotubes, including near-field nonlinear-optical probing and sensing, optical switching, enhanced electromagnetic absorption, and materials nanoscale modification.
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