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Register a new userAbsorption Cross-Section and Near-Field Enhancement in Finite-Length Carbon Nanotubes in the Terahertz-to-Optical Range
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Electromagnetic characteristics of single-walled finite-length carbon nanotubes - absorption cross-section and field enhancement in the near zone - are theoretically studied in a wide frequency range from terahertz to visible. The analysis is based on the impedance-type effective boundary conditions and the integral equation technique. Comparison with experimental results is carried out allowing qualitative physical interpretation of low-frequency (far-IR and terahertz) absorption band observed in experiments. Potentiality of CNTs for the IR photothermolysis of living cells is discussed. Strong local field enhancement is predicted to be inherent to metallic CNTs in the near-field zone providing necessary mechanism for far-IR and terahertz near-field optics.
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The absorption cross section of highly luminescent individual single-walled carbon nanotubes is determined using time-resolved and cw luminescence spectroscopy. A mean value of 1x10-17 cm2 per carbon atom is obtained for (6,5) tubes excited at their second optical transition, and corroborated by single tube photothermal absorption measurements. Biexponential luminescence decays are systematically observed, with short and long lifetimes around 45 and 250 ps. This behavior is attributed to the band edge exciton fine structure with a dark level lying a few meV below a bright one.
We present a detailed study of the vibrational properties of Single Wall Carbon Nanotubes (SWNTs). The phonon dispersions of SWNTs are strongly shaped by the effects of electron-phonon coupling. We analyze the separate contributions of curvature and confinement. Confinement plays a major role in modifying SWNT phonons and is often more relevant than curvature. Due to their one-dimensional character, metallic tubes are expected to undergo Peierls distortions (PD) at T=0K. At finite temperature, PD are no longer present, but phonons with atomic displacements similar to those of the PD are affected by strong Kohn anomalies (KA). We investigate by Density Functional Theory (DFT) KA and PD in metallic SWNTs with diameters up to 3 nm, in the electronic temperature range from 4K to 3000 K. We then derive a set of simple formulas accounting for all the DFT results. Finally, we prove that the static approach, commonly used for the evaluation of phonon frequencies in solids, fails because of the SWNTs reduced dimensionality. The correct description of KA in metallic SWNTs can be obtained only by using a dynamical approach, beyond the adiabatic Born-Oppenheimer approximation, by taking into account non-adiabatic contributions. Dynamic effects induce significant changes in the occurrence and shape of Kohn anomalies. We show that the SWNT Raman G peak can only be interpreted considering the combined dynamic, curvature and confinement effects. We assign the G+ and G- peaks of metallic SWNTs to TO (circumferential) and LO (axial) modes, respectively, the opposite of semiconducting SWNTs.
Excitons play major roles in optical processes in modern semiconductors, such as single-wall carbon nanotubes (SWCNTs), transition metal dichalcogenides, and 2D perovskite quantum wells. They possess extremely large binding energies (>100~meV), dominating absorption and emission spectra even at high temperatures. The large binding energies imply that they are stable, that is, hard to ionize, rendering them seemingly unsuited for optoelectronic devices that require mobile charge carriers, especially terahertz emitters and solar cells. Here, we have conducted terahertz emission and photocurrent studies on films of aligned single-chirality semiconducting SWCNTs and find that excitons autoionize, i.e., spontaneously dissociate into electrons and holes. This process naturally occurs ultrafast (<1~ps) while conserving energy and momentum. The created carriers can then be accelerated to emit a burst of terahertz radiation when a dc bias is applied, with promising efficiency in comparison to standard GaAs-based emitters. Furthermore, at high bias, the accelerated carriers acquire high enough kinetic energy to create secondary excitons through impact exciton generation, again in a fully energy and momentum conserving fashion. This exciton multiplication process leads to a nonlinear photocurrent increase as a function of bias. Our theoretical simulations based on nonequilibrium Boltzmann transport equations, taking into account all possible scattering pathways and a realistic band structure, reproduce all our experimental data semi-quantitatively. These results not only elucidate the momentum-dependent ultrafast dynamics of excitons and carriers in SWCNTs but also suggest promising routes toward terahertz excitonics despite the orders-of-magnitude mismatch between the exciton binding energies and the terahertz photon energies.
We derive the generalized magneto-absorption spectra for curved graphene nanorib- bons and carbon nanotubes by using the Peierls tight-binding model. The main spectral characteristics and the optical selection rules result from the cooperative or competitive relationships between the geometric structure and a magnetic field. In curved ribbons, the dominant selection rule remains unchanged during the variation of the curvature. When the arc angle increases, the prominent peaks are split, with some even vanishing as the angle exceeds a critical value. In carbon nanotubes, the angular-momentum coupling induces extra selection rules, of which more are revealed due to the increase of either (both) of the factors: tube diameter and field strength. Particularly once the two factors exceed certain critical values, the optical spectra could reflect the quasi-Landau-level structures. The identifying features of the spec- tra provide insight into optical excitations for curved systems with either open or closed boundary condition.
The linear polarizability absorption spectra of the double-walled carbon nanotubes (DWNTs) have been calculated by using the tight-binding (TB) model and sum-over-state (SOS) method, supplemented by the first principles CASTEP calculations. It is found that the chiral symmetries of both outer and inner tubes in the DWNTs can always be identified distinctly by the characteristic peaks in the absorption spectra of the DWNTs, no matter what kind of the outer tube is, offering a powerful experimental tool to measure precisely the chiral angle of the inner tube of a DWNT.
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