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Register a new userChirality-Selective Excitation of Coherent Phonons in Carbon Nanotubes
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Using pre-designed trains of femtosecond optical pulses, we have selectively excited coherent phonons of the radial breathing mode of specific-chirality single-walled carbon nanotubes within an ensemble sample. By analyzing the initial phase of the phonon oscillations, we prove that the tube diameter initially increases in response to ultrafast photoexcitation. Furthermore, from excitation profiles, we demonstrate that an excitonic absorption peak of carbon nanotubes periodically oscillates as a function of time when the tube diameter undergoes radial breathing mode oscillations.
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I demonstrate a directional motion-transmission behavior of aligned carbon nanotubes (CNTs) using atomistic simulations. The network of overlapping $pi$ orbitals at the interface act as gear teeth to translate the sliding motion of a CNT into a rotating motion of the adjacent CNT, or textit{viceversa}. The efficiency of this orthogonal motion transmission is found to strongly depend on the tube chirality, by which the interfacial stacking configuration of the atoms is determined. These results have strong implications on the design of the motion transmission system at the nanoscale.
We present a detailed study of the vibrational properties of Single Wall Carbon Nanotubes (SWNTs). The phonon dispersions of SWNTs are strongly shaped by the effects of electron-phonon coupling. We analyze the separate contributions of curvature and confinement. Confinement plays a major role in modifying SWNT phonons and is often more relevant than curvature. Due to their one-dimensional character, metallic tubes are expected to undergo Peierls distortions (PD) at T=0K. At finite temperature, PD are no longer present, but phonons with atomic displacements similar to those of the PD are affected by strong Kohn anomalies (KA). We investigate by Density Functional Theory (DFT) KA and PD in metallic SWNTs with diameters up to 3 nm, in the electronic temperature range from 4K to 3000 K. We then derive a set of simple formulas accounting for all the DFT results. Finally, we prove that the static approach, commonly used for the evaluation of phonon frequencies in solids, fails because of the SWNTs reduced dimensionality. The correct description of KA in metallic SWNTs can be obtained only by using a dynamical approach, beyond the adiabatic Born-Oppenheimer approximation, by taking into account non-adiabatic contributions. Dynamic effects induce significant changes in the occurrence and shape of Kohn anomalies. We show that the SWNT Raman G peak can only be interpreted considering the combined dynamic, curvature and confinement effects. We assign the G+ and G- peaks of metallic SWNTs to TO (circumferential) and LO (axial) modes, respectively, the opposite of semiconducting SWNTs.
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.
From resonant Raman scattering on isolated nanotubes we obtained the optical transition energies, the radial breathing mode frequency and Raman intensity of both metallic and semiconducting tubes. We unambiguously assigned the chiral index (n_1,n_2) of approximately 50 nanotubes based solely on a third-neighbor tight-binding Kataura plot and find omega_RBM=214.4cm^-1nm/d+18.7cm^-1. In contrast to luminescence experiments we observe all chiralities including zig-zag tubes. The Raman intensities have a systematic chiral-angle dependence confirming recent ab-initio calculations.
We study the dependence of thermal conductivity of single walled nanotubes (SWNT) on chirality and isotope impurity by nonequilibrium molecular dynamics method with accurate potentials. It is found that, contrary to electronic conductivity, the thermal conductivity is insensitive to the chirality. The isotope impurity, however, can reduce the thermal conductivity up to 60% and change the temperature dependence behavior. We also study the dependence of thermal conductivity on tube length for tubes of different radius at different temperatures.
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