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Register a new userExciton Dynamics in Carbon Nanotubes: From the Luttinger Liquid to Harmonic Oscillators
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We show that the absorption spectrum in semiconducting nanotubes can be determined using the bosonization technique combined with mean-field theory and a harmonic approximation. Our results indicate that a multiple band semiconducting nanotube reduces to a system of weakly coupled harmonic oscillators. Additionally, the quasiparticle nature of the electron and hole that comprise an optical exciton emerges naturally from the bosonized model.
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An interacting one-dimensional (1D) electron system is predicted to behave very differently than its higher-dimensional counterparts. Coulomb interactions strongly modify the properties away from those of a Fermi liquid, resulting in a Luttinger liquid (LL) characterized by a power-law vanishing of the density of states at the Fermi level. Experiments on one-dimensional semiconductor wires and fractional quantum Hall conductors have been interpreted using this picture, but questions remain about the connection between theory and experiment. Recently, single-walled carbon nanotubes (SWNTs) have emerged as a new type of 1D conductor that may exhibit LL behavior. Here we present measurements of the conductance of individual ropes of such SWNTs as a function of temperature and voltage. Power law behavior as a function of temperature or bias voltage is observed: G~ T^a and dI/dV ~ V^a. Both the power-law functional forms and the inferred exponents are in good agreement with theoretical predictions for tunneling into a LL.
The low-energy theory for multi-wall carbon nanotubes including the long-ranged Coulomb interactions, internal screening effects, and single-electron hopping between graphite shells is derived and analyzed by bosonization methods. Characteristic Luttinger liquid power laws are found for the tunneling density of states, with exponents approaching their Fermi liquid value only very slowly as the number of conducting shells increases. With minor modifications, the same conclusions apply to transport in ropes of single-wall nanotubes.
We study theoretically the interactions of excitonic states with surface electromagnetic modes of small-diameter (~1 nm) semiconducting single-walled carbon nanotubes. We show that these interactions can result in strong exciton-surface-plasmon coupling. The exciton absorption lineshapes exhibit the line (Rabi) splitting $~0.1-0.3$ eV as the exciton energy is tuned to the nearest interband surface plasmon resonance of the nanotube. We expect this effect to open a path to new optoelectronic device applications of semiconducting carbon nanotubes.
We report that dark excitons can have a large contribution to the emission intensity in carbon nanotubes due to an efficient exciton conversion from a dark state to a bright state. Time-resolved photoluminescence measurements are used to investigate decay dynamics and diffusion properties of excitons, and we obtain intrinsic lifetimes and diffusion lengths of bright excitons as well as diffusion coefficients for both bright and dark excitons. We find that the dark-to-bright transition rates can be considerably high, and that more than half of the dark excitons can be transformed into the bright excitons. The state transition rates have a large chirality dependence with a family pattern, and the conversion efficiency is found to be significantly enhanced by adsorbed air molecules on the surface of the nanotubes. Our findings show the nontrivial significance of the dark excitons on the emission kinetics in low dimensional materials, and demonstrate the potential for engineering the dark-to-bright conversion process by using surface interactions.
We propose a framework for inducing strong optomechanical effects in a suspended carbon nanotube based on deformation potential exciton-phonon coupling. The excitons are confined using an inhomogeneous axial electric field which generates optically active quantum dots with a level spacing in the milli-electronvolt range and a characteristic size in the 10-nanometer range. A transverse field induces a tunable parametric coupling between the quantum dot and the flexural modes of the nanotube mediated by electron-phonon interactions. We derive the corresponding excitonic deformation potentials and show that this interaction enables efficient optical ground-state cooling of the fundamental mode and could allow us to realise the strong and ultra-strong coupling regimes of the Jaynes-Cummings and Rabi models.
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