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Register a new userOrganic molecular tuning of many-body interaction energies in air-suspended carbon nanotubes
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We investigate adsorption effects of copper phthalocyanine molecules on excitons and trions in air-suspended carbon nanotubes. Using photoluminescence excitation spectroscopy, we observe that exciton energy redshifts gradually with the molecular deposition thickness. The trion emission is also observed at large deposition amounts, which indicates charge transfer between the phthalocyanine molecules and carbon nanotubes. Analysis of the spectra for individual tubes reveal a correlation between the exciton-trion energy separation and the exciton emission energy, showing that the many-body interaction energies scale similarly with the molecular dielectric screening.
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Organic color centers in single-walled carbon nanotubes have demonstrated exceptional ability to generate single photons at room temperature in the telecom range. Combining the color centers with pristine air-suspended tubes would be desirable for improved performance, but all current synthetic methods occur in solution which makes them incompatible. Here we demonstrate formation of color centers in air-suspended nanotubes using vapor-phase reaction. Functionalization is directly verified on the same nanotubes by photoluminescence spectroscopy, with unambiguous statistics from more than a few thousand individual nanotubes. The color centers show a strong diameter-dependent emission intensity, which can be explained with a theoretical model for chemical reactivity taking into account strain along the tube curvature. We are also able to estimate the defect density by comparing the experiments with simulations based on a one-dimensional diffusion equation, whereas the analysis of diameter dependent peak energies gives insight to the nature of the dopant states. Time-resolved measurements show a longer lifetime for color center emission compared to E$_{11}$ exciton states. Our results highlight the influence of the tube structure on vapor-phase reactivity and emission properties, providing guidelines for development of high-performance near-infrared quantum light sources.
The electronic Raman scattering (ERS) features of single-walled carbon nanotubes (SWNTs) can reveal a wealth of information about their electronic structures, but have previously been thought to appear exclusively in metallic (M-) but not in semiconducting (S-) SWNTs. We report the experimental observation of the ERS features with an accuracy of 1 meV in suspended S-SWNTs, the processes of which are accomplished via the available high-energy electron-hole pairs. The ERS features can facilitate further systematic studies on the properties of SWNT, both metallic and semiconducting, with defined chirality.
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 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.
Current-voltage characteristics of suspended single-wall carbon nanotube quantum dots show a series of steps equally spaced in voltage. The energy scale of this harmonic, low-energy excitation spectrum is consistent with that of the longitudinal low-k phonon mode (stretching mode) in the nanotube. Agreement is found with a Franck-Condon-based model in which the phonon-assisted tunneling process is modeled as a coupling of electronic levels to underdamped quantum harmonic oscillators. Comparison with this model indicates a rather strong electron-phonon coupling factor of order unity.
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