This Letter reports the laser energy dependence of the Stokes and anti-Stokes Raman spectra of carbon nanotubes dispersed in aqueous solution and within solid bundles, in the energy range 1.52-2.71 eV. The electronic transition energies (E(ii)) and the radial breathing mode frequencies (omega(RBM)) are obtained for 46 different (18 metallic and 28 semiconducting) nanotubes, and the (n,m) assignment is discussed based on the observation of geometrical patterns for E(ii) versus omega(RBM) graphs. Only the low energy component of the E(M)(11) value is observed from each metallic nanotube. For a given nanotube, the resonant window is broadened and down-shifted for single wall carbon nanotube (SWNT) bundles compared to SWNTs in solution, while by increasing the temperature, the E(S)(22) energies are redshifted for S1 [(2n+m) mod 3=1] nanotubes and blueshifted for S2 [(2n+m) mod 3=2] nanotubes.
Double-resonance Raman scattering is a sensitive probe to study the electron-phonon scattering pathways in crystals. For semiconducting two-dimensional transition-metal dichalcogenides, the double-resonance Raman process involves different valleys and phonons in the Brillouin zone, and it has not yet been fully understood. Here we present a multiple energy excitation Raman study in conjunction with density functional theory calculations that unveil the double-resonance Raman scattering process in monolayer and bulk MoS2. Results show that the frequency of some Raman features shifts when changing the excitation energy, and first-principle simulations confirm that such bands arise from distinct acoustic phonons, connecting different valley states. The double-resonance Raman process is affected by the indirect-to-direct bandgap transition, and a comparison of results in monolayer and bulk allows the assignment of each Raman feature near the M or K points of the Brillouin zone. Our work highlights the underlying physics of intervalley scattering of electrons by acoustic phonons, which is essential for valley depolarization in MoS2.
Resonant Raman spectroscopy (RRS) is a very useful tool to study physical properties of materials since it provides information about excitons and their coupling with phonons. We present in this work a RRS study of samples of WSe2 with one, two, and three layers (1L, 2L, and 3L), as well as bulk 2H-WSe2, using up to 20 different laser lines covering the visible range. The first- and second-order Raman features exhibit different resonant behavior, in agreement with the double (and triple) resonance mechanism(s). From the laser energy dependence of the Raman intensities (Raman excitation profile, or REP), we obtained the energies of the excited excitonic states and their dependence with the number of atomic layers. Our results show that Raman enhancement is much stronger for the excited A' and B' states, and this result is ascribed to the different exciton-phonon coupling with fundamental and excited excitonic states.
This paper presents an accurate analysis of ͑i͒ the electronic transition energies E 22 S and E 11 M , ͑ii͒ the radial breathing mode ͑RBM͒ frequencies RBM , and ͑iii͒ the corresponding RBM intensities from 40 small-diameter single-wall carbon nanotubes ͑SWNTs͒ in the diameter range 0.7Ͻ d t Ͻ 1.3 nm. The electronic transition energies ͑E ii ͒ are initially considered from nonorthogonal tight-binding total-energy calculations. To account for d t -dependent many-body effects, a logarithmic correction, as proposed by Kane and Mele, is applied to both E 22 S and E 11 M . The remaining discrepancies between the experimental and theoretical E ii values are shown to beproportional to the chirality-dependent effective masses of electrons and holes, as obtained from the electron energy dispersion relations. Chirality dependent screening effects are also identified in metallic SWNTs. For the RBM frequencies, a small deviation from the linear 1 / d t behavior is observed, and this deviation is analyzed based on a chirality-dependent mode softening effect due to nanotube curvature. For those interested in sample characterization, the ͑n , m͒ dependence of the resonance intensities is also addressed, the experimental results being compared with theoretical predictions based on matrix elements calculations. This analysis suggests that the ͑7,5͒, ͑7,6͒, and ͑6,5͒ SWNTs are more abundant in sodium dodecyl sulfate wrapped HiPco SWNTs in aqueous solution, in agreement with results previously reported for SWNTs grown by the CoMoCAT or alcohol methods.
The method for quantifying the amount of each carbon nanotube specie, as defined by its diameter and chiral angle, as well as the semiconducting-to-metallic ratio in any type of carbon nanotube sample is discussed. Single-wall carbon nanotubes grown by the cobalt-molybdenum catalyst based ͑CoMoCAT͒ process are characterized. The semiconducting-to-metallic ratio is found to be 11:1. A single semiconducting specie, named the ͑6,5͒ nanotube represents 2 / 5 of the sample, while the most abundant metallic nanotube is the ͑7,4͒, which exhibits a diameter similar to the ͑6,5͒.
This work describes a resonance Raman study performed on samples with one, two, and three layers (1L, 2L, 3L), and bulk MoS2, using more than 30 different laser excitation lines covering the visible range, and focusing on the intensity of the two most pronounced features of the Raman scattering spectrum of MoS2 (E2g(1) and A1g bands). The Raman excitation profiles of these bands were obtained experimentally, and it is found that the A1g feature is enhanced when the excitation laser is in resonance with A and B excitons of MoS2, while the E2g1 feature is shown to be enhanced when the excitation laser is close to 2.7 eV. We show from the symmetry analysis of the exciton-phonon interaction that the mode responsible for the E2g(1) resonance is identified as the high energy C exciton recently predicted [D. Y. Qiu, F. H. da Jornada, and S. G. Louie, Phys. Rev. Lett. 111, 216805 (2013)].
In this work we analyze the room-temperature linewidth for several Raman features ͑i.e., the radial breathing mode, the G band, the D band, and the GЈ band͒ observed for individual isolated single-wall carbon nanotubes ͑SWNTs͒. Temperature-dependent measurements on SWNT bundles and isolated SWNTs show that anharmonic effects are not important for linewidth broadening at room temperature. Measurements on a large number of samples ͑170 isolated SWNTs͒ allow us to filter out the effect from extrinsic SWNT properties ͑e.g., defects, tube deformations, substrate roughness͒ and to obtain information about intrinsic properties related to phonon and electron dispersion relations, curvature and Breit-Wigner-Fano effects, single-vs double-resonance Raman scattering processes, and the resonance condition itself through a linewidth analysis. We also use observations at the single-nanotube level to understand linewidth effects in SWNT bundles.
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