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Register a new userBinding Energy and Lifetime of Excitons in Metallic Nanotubes
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The difficulty of describing excitons in semiconducting SWNTs analytically lies with the fact that excitons can neither be considered strictly 1D nor 2D objects. However, the situation changes in the case of metallic nanotubes where, by virtue of screening from gapless metallic subbands, the radius of the exciton becomes much larger than the radius of the nanotube $R_text{ex}gg R$. Taking advantage of this, we develop the theory of excitons in metallic nanotubes, determining that their binding energy is about $0.08v/R$, in agreement with the existing experimental data. Additionally, because of the presence of the gapless subbands, there are processes where bound excitons are scattered into unbound electron-hole pairs belonging to the gapless subbands. Such processes lead to a finite exciton lifetime and the broadening of its spectral function. We calculate the corresponding decay rate of the excitons.
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We calculate the radiative lifetime and energy bandstructure of excitons in semiconducting carbon nanotubes, within a tight-binding approach. In the limit of rapid interband thermalization, the radiative decay rate is maximized at intermediate temperatures, decreasing at low temperature because the lowest-energy excitons are optically forbidden. The intrinsic phonons cannot scatter excitons between optically active and forbidden bands, so sample-dependent extrinsic effects that break the symmetries can play a central role. We calculate the diameter-dependent energy splittings between singlet and triplet excitons of different symmetries, and the resulting dependence of radiative lifetime on temperature and tube diameter.
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.
Single-layer transition metal dichalcogenides (TMDs) provide a promising material system to explore the electrons valley degree of freedom as a quantum information carrier. The valley degree of freedom in single-layer TMDs can be directly accessed by means of optical excitation. The rapid valley relaxation of optically excited electron-hole pairs (excitons) through the long-range electron-hole exchange interaction, however, has been a major roadblock. Theoretically such a valley relaxation does not occur for the recently discovered dark excitons, suggesting a potential route for long valley lifetimes. Here we investigate the valley dynamics of dark excitons in single-layer WSe2 by time-resolved photoluminescence spectroscopy. We develop a waveguide-based method to enable the detection of the dark exciton emission, which involves spin-forbidden optical transitions with an out-of-plane dipole moment. The valley degree of freedom of dark excitons is accessed through the valley-dependent Zeeman effect under an out-of-plane magnetic field. We find a short valley lifetime for the dark neutral exciton, likely due to the short-range electron-hole exchange, but long valley lifetimes exceeding several nanoseconds for dark charged excitons.
We have studied the discrete electronic spectrum of closed metallic nanotube quantum dots. At low temperatures, the stability diagrams show a very regular four-fold pattern that allows for the determination of the electron addition and excitation energies. The measured nanotube spectra are in excellent agreement with theoretical predictions based on the nanotube band structure. Our results permit the complete identification of the electron quantum states in nanotube quantum dots.
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.
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