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تسجيل مستخدم جديدElectrical generation and absorption of phonons in carbon nanotubes
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The interplay between discrete vibrational and electronic degrees of freedom directly influences the chemical and physical properties of molecular systems. This coupling is typically studied through optical methods such as fluorescence, absorption, and Raman spectroscopy. Molecular electronic devices provide new opportunities for exploring vibration-electronic interactions at the single molecule level. For example, electrons injected from a scanning tunneling microscope tip into a metal can excite vibrational excitations of a molecule in the gap between tip and metal. Here we show how current directly injected into a freely suspended individual single-wall carbon nanotube can be used to excite, detect, and control a specific vibrational mode of the molecule. Electrons inelastically tunneling into the nanotube cause a non-equilibrium occupation of the radial breathing mode, leading to both stimulated emission and absorption of phonons by successive electron tunneling events. We exploit this effect to measure a phonon lifetime on the order of 10 nanoseconds, corresponding to a quality factor well over 10000 for this nanomechanical oscillator.
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We review recent studies of coherent phonons (CPs) corresponding to the radial breathing mode (RBM) and G-mode in single-wall carbon nanotubes (SWCNTs) and graphene. Because of the bandgap-diameter relationship, RBM-CPs cause bandgap oscillations in
SWCNTs, modulating interband transitions at terahertz frequencies. Interband resonances enhance CP signals, allowing for chirality determination. Using pulse shaping, one can selectively excite speci!c-chirality SWCNTs within an ensemble. G-mode CPs exhibit temperature-dependent dephasing via interaction with RBM phonons. Our microscopic theory derives a driven oscillator equation with a density-dependent driving term, which correctly predicts CP trends within and between (2n+m) families. We also find that the diameter can initially increase or decrease. Finally, we theoretically study the radial breathing like mode in graphene nanoribbons. For excitation near the absorption edge, the driving term is much larger for zigzag nanoribbons. We also explain how the armchair nanoribbon width changes in response to laser excitation.
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.
We study theoretically the impact of Zener tunneling on the charge-transport properties of quasi-metallic (Qm) carbon nanotubes (characterized by forbidden band gaps of few tens of meV). We also analyze the interplay between Zener tunneling and elast
ic scattering on defects. To this purpose we use a model based on the master equation for the density matrix, that takes into account the inter-band Zener transitions induced by the electric field (a quantum mechanical effect), the electron-defect scattering and the electron-phonon scattering. In presence of Zener tunnelling the Qm tubes support an electrical current even when the Fermi energy lies in the forbidden band gap. In absence of elastic scattering (in high quality samples), the small size of the band gap of Qm tubes enables Zener tunnelling for realistic values of the the electric field (above $sim$ 1 V/mu m). The presence of a strong elastic scattering (in low quality samples) further decreases the values of the field required to observe Zener tunnelling. Indeed, for elastic-scattering lengths of the order of 50 nm, Zener tunnelling affects the current/voltage characteristic already in the linear regime. In other words, in quasi-metallic tubes, Zener tunneling is made more visible by defects.
The transport properties of a suspended carbon nanotube probed by means of a STM tip are investigated. A microscopic theory of the coupling between electrons and mechanical vibrations is developed. It predicts a position-dependent coupling constant,
sizeable only in the region where the vibron is located. This fact has profound consequences on the transport properties, which allow to extract information on the location and size of the vibrating portions of the nanotube.
We have used a femtosecond pump-probe impulsive Raman technique to explore the polarization dependence of coherent optical phonons in highly-purified and aligned semiconducting single-wall carbon nanotubes (SWCNTs). Coherent phonon spectra for the ra
dial breathing modes (RBMs) exhibit a different monochromatic frequency between the film and solution samples, indicating the presence of differing exciton excitation processes. By varying the polarization of the incident pump beam on the aligned SWCNT film, we found that the anisotropy of the coherent RBM excitation depends on the laser wavelength, which we consider to be associated with the resonant and off-resonant behavior of RBM excitation.
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