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Register a new userDirect Observation of Cross-Polarized Excitons in Aligned Single-Chirality Single-Wall Carbon Nanotubes
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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.
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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.
We report the observation of strong third harmonic generation from a macroscopic array of aligned ultralong single-wall carbon nanotubes (SWCNTs) with intense midinfrared radiation. Through power-dependent experiments, we determined the absolute value of the third-order nonlinear optical susceptibility, $chi^{(3)}$, of our SWCNT film to be 5.53 $times$ 10$^{-12}$ esu, three orders of magnitude larger than that of the fused silica reference we used. Taking account of the filling factor of 8.75% for our SWCNT film, we estimate a $chi^{(3)}$ of 6.32 $times$ 10$^{-11}$ esu for a fully dense film. Furthermore, through polarization-dependent experiments, we extracted all the nonzero elements of the $chi^{(3)}$ tensor, determining the magnitude of the weaker tensor elements to be $sim$1/6 of that of the dominant $chi^{(3)}_{zzzz}$ component.
Ultrafast terahertz spectroscopy accesses the {em dark} excitonic ground state in resonantly-excited (6,5) SWNTs via internal, direct dipole-allowed transitions between lowest lying dark-bright pair state $sim$6 meV. An analytical model reproduces the response which enables quantitative analysis of transient densities of dark excitons and {em e-h} plasma, oscillator strength, transition energy renormalization and dynamics. %excitation-induced renormalization. Non-equilibrium, yet stable, quasi-1D quantum states with dark excitonic correlations rapidly emerge even with increasing off-resonance photoexcitation and experience a unique crossover to complex phase-space filling of %a complex distribution between both dark and bright pair states, different from dense 2D/3D excitons influenced by the thermalization, cooling and ionization to free carriers.
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.
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.
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