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Register a new userExcitons and high-order optical transitions in individual carbon nanotubes
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We examine the excitonic nature of high-lying optical transitions in single-walled carbon nanotubes by means of Rayleigh scattering spectroscopy. A careful analysis of the principal transitions of individual semiconducting and metallic nanotubes reveals that in both cases the lineshape is consistent with an excitonic model, but not one of free-carriers. For semiconducting species, side-bands are observed at ~200 meV above the third and fourth optical transitions. These features are ascribed to exciton-phonon bound states. Such side-bands are not apparent for metallic nanotubes,as expected from the reduced strength of excitonic interactions in these systems.
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We report the direct observation of the spin-singlet dark excitonic state in individual single-walled carbon nanotubes through low-temperature micro-photoluminescence spectroscopy in magnetic fields. A magnetic field up to 5 T, applied along the nanotube axis, brightened the dark state, leading to the emergence of a new emission peak. The peak rapidly grew in intensity with increasing field at the expense of the originally-dominant bright exciton peak and finally became dominant at fields $>$3 T. This behavior, universally observed for more than 50 nanotubes of different chiralities, can be quantitatively explained through a model incorporating the Aharonov-Bohm effect and intervalley Coulomb mixing, unambiguously proving the existence of dark excitons. The directly measured dark-bright splitting values were 1-4 meV for tube diameters 1.0-1.3 nm. Scatter in the splitting value emphasizes the role of the local environment surrounding a nanotube in determining the excitonic fine structure of single-walled carbon nanotubes.
Through ultrafast pump-probe spectroscopy with intense pump pulses and a wide continuum probe, we show that interband exciton peaks in single-walled carbon nanotubes (SWNTs) are extremely stable under high laser excitations. Estimates of the initial densities of excitons from the excitation conditions, combined with recent theoretical calculations of exciton Bohr radii for SWNTs, suggest that their positions do not change at all even near the Mott density. In addition, we found that the presence of lowest-subband excitons broadens all absorption peaks, including those in the second-subband range, which provides a consistent explanation for the complex spectral dependence of pump-probe signals reported for SWNTs.
Near-infrared magneto-optical spectroscopy of single-walled carbon nanotubes reveals two absorption peaks with an equal strength at high magnetic fields ($>$ 55 T). We show that the peak separation is determined by the Aharonov-Bohm phase due to the tube-threading magnetic flux, which breaks the time-reversal symmetry and lifts the valley degeneracy. This field-induced symmetry breaking thus overcomes the Coulomb-induced intervalley mixing which is predicted to make the lowest exciton state optically inactive (or ``dark).
The efficiencies of photonic devices are primarily governed by radiative quantum efficiency, which is a property given by the light emitting material. Quantitative characterization for carbon nanotubes, however, has been difficult despite being a prominent material for nanoscale photonics. Here we determine the radiative quantum efficiency of bright excitons in carbon nanotubes by modifying the exciton dynamics through cavity quantum electrodynamical effects. Silicon photonic crystal nanobeam cavities are used to induce the Purcell effect on individual carbon nanotubes. Spectral and temporal behavior of the cavity enhancement is characterized by photoluminescence microscopy, and the fraction of the radiative decay process is evaluated. We find that the radiative quantum efficiency is near unity for bright excitons in carbon nanotubes at room temperature.
We use the robust nearest-neighbour tight-binding approximation to study on the same footing interband dipole transitions in narrow-bandgap carbon nanotubes and graphene nanoribbons. It is demonstrated that curvature effects in metallic single-walled carbon nanotubes and edge effects in gapless graphene nanoribbons not only open up bang gaps, which typically correspond to THz frequencies, but also result in a giant enhancement of the probability of optical transitions across these gaps. Moreover, the matrix element of the velocity operator for these transitions has a universal value (equal to the Fermi velocity in graphene) when the photon energy coincides with the band-gap energy. Upon increasing the excitation energy, the transition matrix element first rapidly decreases (for photon energies remaining in the THz range but exceeding two band gap energies it is reduced by three orders of magnitude), and thereafter it starts to increase proportionally to the photon frequency. A similar effect occurs in an armchair carbon nanotube with a band gap opened and controlled by a magnetic field applied along the nanotube axis. There is a direct correspondence between armchair graphene nanoribbons and single-walled zigzag carbon nanotubes. The described sharp photon-energy dependence of the transition matrix element together with the van Hove singularity at the band gap edge of the considered quasi-one-dimensional systems make them promising candidates for active elements of coherent THz radiation emitters. The effect of Pauli blocking of low-energy interband transitions caused by residual doping can be suppressed by creating a population inversion using high-frequency (optical) excitation.
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