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Register a new userHigh efficiency dark-to-bright exciton conversion in carbon nanotubes
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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.
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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 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.
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.
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.
In cavity quantum electrodynamics, optical emitters that are strongly coupled to cavities give rise to polaritons with characteristics of both the emitters and the cavity excitations. We show that carbon nanotubes can be crystallized into chip-scale, two-dimensionally ordered films and that this new material enables intrinsically ultrastrong emitter-cavity interactions: rather than interacting with external cavities, nanotube excitons couple to the near-infrared plasmon resonances of the nanotubes themselves. Our polycrystalline nanotube films have a hexagonal crystal structure, ~25 nm domains, and a 1.74 nm lattice constant. With this extremely high nanotube density and nearly ideal plasmon-exciton spatial overlap, plasmon-exciton coupling strengths reach 0.5 eV, which is 75% of the bare exciton energy and a near record for room-temperature ultrastrong coupling. Crystallized nanotube films represent a milestone in nanomaterials assembly and provide a compelling foundation for high-ampacity conductors, low-power optical switches, and tunable optical antennas.
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