Spectra of radiation emitted by single-walled and multi-walled carbon nanotubes during multiple microwave irradiation and cooling cycles
S. Ferguson, N. McGara, B. Cavness, D. Gonzales, S. Williams
备注：
This paper has been withdrawn by the authors. Although the experimental data presented in this paper is sound, the interpretation of the data presented in the paper is now believed to be incorrect
发表信息：
International Journal of Nanoscience and Nanotechnology 4 (2013), pp. 71-79
Carbon nanotubes have been observed to emit ultraviolet, visible, and infrared radiation when exposed to microwave fields. We have performed experiments in which both single-walled (~1 nm diameters) and multi-walled carbon nanotubes (>50 nm diameters) were exposed to 2.45 GHz microwaves during several irradiation and cooling cycles at a pressure of ~10-6 torr. A comparison of the spectra of the radiation emitted by the nanotubes indicates that the intensity of radiation with wavelengths ranging from 700 to 1000 nm increased substantially during the course of five irradiation and cooling cycles. The data suggests that the mechanism responsible for the emissions is field emission-induced luminescence and that the intensity of the radiation emitted increased due to the opening of nanotube ends. Furthermore, the intensity of the radiation emitted by the multi-walled carbon nanotubes was much greater than the radiation emitted by the single-walled nanotubes. Scanning electron microscopy images indicate that most of the single-walled nanotubes were bundled together, while the multi-walled nanotubes were not. This bundling may have resulted in a lower field enhancement factor and/or screening effects which might help to explain the difference in the intensities of the radiation emitted by the samples.
Single- and multi-walled molybdenum disulfide (MoS$_2$) nanotubes have been coaxially grown on small diameter boron nitride nanotubes (BNNTs) which were synthesized from heteronanotubes by removing single-walled carbon nanotubes (SWCNTs), and systematically investigated by optical spectroscopy. The strong photoluminescence (PL) from single-walled MoS$_2$ nanotubes supported by core BNNTs is observed in this work, which evidences a direct band gap structure for single-walled MoS$_2$ nanotubes with around 6 - 7 nm in diameter. The observation is consistent with our DFT results that the single-wa…
A simple method to disperse individual single walled carbon nanotubes (SWCNT ) on an atomically flat substrate is presented. Proper tuning of ac modes of atomic force microscopes(AFM) is discussed. This is needed to discriminate between individual nanotubes and very small bundles. The distribution of lengths of the nanotubes measured by these methods is reported.
The ability to integrate carbon nanotubes, especially single-walled carbon nanotubes, seamlessly onto silicon would expand the range of applications considerably. Though direct integration using chemical vapor deposition is the simplest method, the growth of single-walled carbon nanotubes on bare silicon and on ultra-thin oxides is greatly inhibited due to the formation of a non-catalytic silicide. Using x-ray photoelectron spectroscopy, we show that silicide formation occurs on ultra-thin oxides due to thermally activated metal diffusion through the oxide. Silicides affect the growth of singl…
We have computed the adsorption of Krypton in a closed single-walled carbon nanotube using the method of Grand Canonical Monte Carlo. Our results indicate evidence of an incommensurate solid formed at high pressure and low temperature (T<85K), before the formation of a second layer. The solid melts above that temperature. Our simulations are in good agreement with novel experimental results for adsorption in individual carbon nanotubes.
Interaction of single-walled carbon nanotubes with electron donor and acceptor molecules causes significant changes in the electronic and Raman spectra, the relative proportion of the metallic species increasing on electron donation through molecular charge transfer, as also verified by electrical resistivity measurements.
We report on the characterization of torsional oscillators which use multi-walled carbon nanotubes as the spring elements. Through atomic-force-microscope force-distance measurements we are able to apply torsional strains to the nanotubes and measure their torsional spring constants and effective shear moduli. We find that the effective shear moduli cover a broad range, with the largest values near the theoretically predicted value. The data also suggest that the nanotubes are stiffened by repeated flexing.
The chemisorption of atomic hydrogen on the single-walled armchair carbon nanotube is studied with ab initio calculations. A single H atom is found to be chemisorbed on both the inside and outside wall of the nanotube. The binding energy of H adsorption at the exterior of the nanotube is much greater than that at the interior of the nanotube. For the first time, we predict that two rows of H atoms chemisorbed on selective sites exterior to the nanotube can break the nearest-neighbor C-C bond of the nanotube through the concerted formation of C-H bonds, leading to the unzipping of the nanotube …
We present a quantitative theory of optical absorption polarized transverse to the tube axes in semiconducting single-walled carbon nanotubes. Transverse optical absorption in semiconducting single-walled carbon nanotubes is to an exciton state that is strongly blueshifted, relative to the two lowest longitudinal excitons, by electron-electron interactions. The binding energy of the transverse exciton is considerably smaller than those of the longitudinal excitons. Electron-electron interactions also reduce the relative oscillator strength of the transverse optical absorption. Our theoretical …
Interactions between atoms of bound single-walled carbon nanotubes (SWNTs) are known to cause measurable distortion to the tube's original circular cross-section frame. High-resolution transmission electron microscope (TEM) investigation was used here to directly image and verify these radial deformations. The data presented here provide, for the first time, direct measurements of the deformations due to the interactions between isolated pairs of nanotubes. The deformation data is compared to previously reported experimental and simulation results.
We present a detailed electron diffraction study of individual single-walled carbon nanotubes. A novel sample preparation procedure provides well-separated, long and straight individual single-shell nanotubes. Diffraction experiments are carried out at 60kV, below the threshold for knock-on damage in carbon nanotubes. We describe experimental parameters that allow single-tube electron diffraction experiments with widely available thermal emission transmission electron microscopes. Further, we review the simulation of diffraction patterns for these objects.
A new molecular motor is conceptually constructed from a double-walled carbon nanotube (DWNT) consisting of a long inner single-walled carbon nanotube (SWNT) and a short outer SWNT with different chirality. The interaction between inner and outer tubes is the sum of the Lennard-Jones potentials between carbon atoms in inner tube and those in outer one. Within the framework of Smoluchowski-Feynman ratchet, it is theoretically shown that this system in an isothermal bath will exhibit a unidirectional rotation in the presence of a varying axial electrical voltage.
We report first-principles calculations of the effects of quasiparticle self-energy and electron-hole interaction on the optical properties of single-walled BN nanotubes. Excitonic effects are shown to be even more important in BN nanotubes than in carbon nanotubes. Electron-hole interactions give rise to complexes of bright (and dark) excitons, which qualitatively alter the optical response. Excitons with binding energy larger than 2 eV are found in the (8,0) BN nanotubes. Moreover, unlike the carbon nanotubes, theory predicts that these exciton states are comprised of coherent supposition of…
Using the first-principles spin density functional approach, we have studied magnetism of a new type of all-carbon nanomaterials, i.e., the carbon nanowires inserted into the single-walled carbon nanotubes. It is found that if the 1D carbon nanowire density is not too higher, the ferromagnetic ground state will be more stable than the antiferromagnetic one, which is caused by weak coupling between the 1D carbon nanowire and the single-walled carbon nanotube. Also, both dimerization of the carbon nanowire and carbon vacancy on the tube-wall are found to enhance the magnetic moment of the compos…
A parametric study of so-called "super growth" of single-walled carbon nanotubes(SWNTs) was done by using combinatorial libraries of iron/aluminum oxide catalysts. Millimeter-thick forests of nanotubes grew within 10 min, and those grown by using catalysts with a thin Fe layer (about 0.5 nm) were SWNTs. Although nanotube forests grew under a wide range of reaction conditions such as gas composition and temperature, the window for SWNT was narrow. Fe catalysts rapidly grew nanotubes only when supported on aluminum oxide. Aluminum oxide, which is a well-known catalyst in hydrocarbon reforming, p…
We report correlated-electron calculations of optically excited states in ten semiconducting single-walled carbon nanotubes with a wide range of diameters. Optical excitation occurs to excitons whose binding energies decrease with the increasing nanotube diameter, and are smaller than the binding energy of an isolated strand of poly-(paraphenylene vinylene). The ratio of the energy of the second optical exciton polarized along the nanotube axis to that of the lowest exciton is smaller than the value predicted within single-particle theory. The experimentally observed weak photoluminescence is …
Single-walled carbon nanotubes are strongly correlated systems with large Coulomb repulsion between two electrons occupying the same $p_z$ orbital. Within a molecular Hamiltonian appropriate for correlated $π$-electron systems, we show that optical excitations polarized parallel to the nanotube axes in the so-called metallic single-walled carbon nanotubes are to excitons. Our calculated absolute exciton energies in twelve different metallic single-walled carbon nanotubes, with diameters in the range 0.8 - 1.4 nm, are in nearly quantitative agreement with experimental results. We have also calc…
Optical limiting behaviour of suspensions of single-walled carbon nanotubes in water, ethanol and ethylene glycol is reported. Experiments with 532 nm, 15 nsec duration laser pulses show that optical limiting occurs mainly due to nonlinear scattering. The observed host liquid dependence of optical limiting in different suspensions suggests that the scattering originates from microbubbles formed due to absorption-induced heating.
It is important to understand the electronic interaction between single-walled carbon nanotubes (SWNTs) and graphene in order to use them efficiently in multifunctional hybrid devices. Here we deposited SWNT bundles on graphene-covered copper and SiO2 substrates by chemical vapor deposition and investigated the charge transfer between them by Raman spectroscopy. Our results revealed that, on both copper and SiO2 substrates, graphene donates electrons to the SWNTs, resulting in p-type doped graphene and n-type doped SWNTs.
Our study of the adsorption of oxygen molecules on individual semiconductiong single-walled carbon nanotubes at ambient conditions reveals that the adsorption is physisorption, that the resistance without O2 increases by ~two orders of magnitude as compared to that with O2, and that the sensitive response is due to the pinning of the Fermi level near the top of the valence band of the tube resulting from impurity states of O2 appearing above the valence band.
We develop a continuous theory of low-frequency dynamics for nanotubes with truly two-dimensional (2D) walls constituted by single-atom monolayer. In this frame topological bending elasticity of the monolayer is not related to its vanishing macroscopic thickness. The proposed approach predicts completely new sound dispersions and radius dependences of non-resonant Raman-active modes frequencies in single-walled carbon nanotubes (SWCNT). Resulting relations are suitable for nanotubes identification and more complete or alternative characterization. The theory is also applied to describe the low…
We investigate experimentally the transport properties of single-walled carbon nanotube bundles as a function of temperature and applied current over broad intervals of these variables. The analysis is performed on arrays of nanotube bundles whose axes are aligned along the direction of the externally supplied bias current. The data are found consistent with a charge transport model governed by the tunnelling between metallic regions occurring through potential barriers generated by nanotubes contact areas or bundles surfaces. Based on this model and on experimental data we describe quantitati…
Diffusion Monte Carlo calculations on the adsorption of $^4$He in open-ended single walled (10,10) nanotubes are presented. We have found a first order phase transition separating a low density liquid phase in which all $^4$He atoms are adsorbed close to the tube wall and a high density arrangement characterized by two helium concentric layers. The energy correction due to the presence of neighboring tubes in a bundle has also been calculated, finding it negligible in the density range considered.
We show by ab initio calculations that the electron-phonon coupling matrix element M of the radial breathing mode in single-walled carbon nanotubes depends strongly on tube chirality. For nanotubes of the same diameter the coupling strength |M|^2 is up to one order of magnitude stronger for zig-zag than for armchair tubes. For (n,m) tubes M depends on the value of (n-m) mod 3, which allows to discriminate semiconducting nano tubes with similar diameter by their Raman scattering intensity. We show measured resonance Raman profiles of the radial breathing mode which support our theoretical predi…
We report benchmark calculations of electroabsorption in semiconducting single-walled carbon nanotubes to provide motivation to experimentalists to perform electroabsorption measurement on these systems. We show that electroabsorption can detect continuum bands in different energy manifolds, even as other nonlinear absorption measurements have failed to detect them. Direct determination of the binding energies of excitons in higher manifolds thereby becomes possible. We also find that electroabsorption can provide evidence for Fano-type coupling between the second exciton and the lowest contin…
Boron-doped multi-walled carbon nanotubes (MWNTs) were synthesized using a methanol solution of boric acid as a source material. Accurate measurements of the electrical resistivity of an individual boron-doped MWNT was performed with a four-point contact, which was fabricated using an electron beam lithography technique. The doped boron provides conduction carriers, which reduces the resistivity of the MWNT.
We studied the asymmetry between valence and conduction bands in single-walled carbon nanotubes (SWNTs) through the direct observation of spin-singlet transverse dark excitons using polarized photoluminescence excitation spectroscopy. The intrinsic electron-hole (e-h) asymmetry lifts the degeneracy of the transverse exciton wavefunctions at two equivalent K and K' valleys in momentum space, which gives finite oscillator strength to transverse dark exciton states. Chirality-dependent spectral weight transfer to transverse dark states was clearly observed, indicating that the degree of the e-h a…
The properties of excitons in semiconducting single-walled carbon nanotubes (SWCNTs), isolated in vacuum or a medium, and their contributions to the optical spectra of nanotubes are studied within the elementary potential model, in which an exciton is represented as a bound state of two oppositely charged quasi-particles confined to the nanotube surface. The emphasis is given on the influence of dielectric environment surrounding a nanotube on the exciton spectra. For nanotubes in environment with permittivity less than 1.8 the ground-state exciton binding energies exceed the respective energy…
In the present work we report significant enhancement of the photoelectrochemical properties of self-organized TiO2 nanotubes by a combined de-coring of classic nanotubes followed by an appropiate TiCl4-treatment. We show that, except for the expected particle decoration, a key effect of the TiCl4 treatment is that the electron transport characteristics in TiO2 nanotubes can be drastically improved, e.g. we observe an enhancement of up to 70 % in electron transport times.
The photovoltaic properties of carbon nanotube/Si heterojunction solar cells were investigated using network films of high quality single-walled carbon nanotubes (SWNTs) grown by atmospheric-pressure floating-catalyst chemical vapor deposition. Because of the optimization of the device window size and the utilization of SWNT thin films with both low resistivity and high transparency, a high photovoltaic conversion efficiency of greater than 12% was achieved for SWNTs/Si heterojunction solar cells without any post processing, such as carrier doping treatment. In addition, the high stability and…
The absorption cross section of highly luminescent individual single-walled carbon nanotubes is determined using time-resolved and cw luminescence spectroscopy. A mean value of 1x10-17 cm2 per carbon atom is obtained for (6,5) tubes excited at their second optical transition, and corroborated by single tube photothermal absorption measurements. Biexponential luminescence decays are systematically observed, with short and long lifetimes around 45 and 250 ps. This behavior is attributed to the band edge exciton fine structure with a dark level lying a few meV below a bright one.
Many-electron effects often dramatically modify the properties of reduced dimensional systems. We report calculations, based on an many-electron Green's function approach, of electron-hole interaction effects on the optical spectra of small-diameter single-walled carbon nanotubes. Excitonic effects qualitatively alter the optical spectra of both semiconducting and metallic tubes. Excitons are bound by ~ 1 eV in the semiconducting (8,0) tube and by ~ 100 meV in the metallic (3,3) tube. These large many-electron effects explain the discrepancies between previous theories and experiments.
Using Coulomb correlation parameters appropriate for $π$-conjugated polymers (PCPs), and a nearest neighbor hopping integral that is arrived at by fitting the energy spectra of three zigzag semiconducting single-walled carbon nanotubes (S-SWCNTs), we are able to determine quantitatively the exciton energies and exciton binding energies of 29 S-SWCNTs within a semiempirical $π$-electron Hamiltonian that has been widely used for PCPs. Our work establishes the existence of a deep and fundamental relationship between PCPs and S-SWCNTs.
Single-walled carbon nanotubes (SWNTs) are typically long (>100 nm) and have been well established as novel quasi one-dimensional systems with interesting electrical, mechanical, and optical properties. Here, quasi zero-dimensional SWNTs with finite lengths down to the molecular scale (7.5 nm in average) were obtained by length separation using a density gradient ultracentrifugation method. Different sedimentation rates of nanotubes with different lengths in a density gradient were taken advantage of to sort SWNTs according to length. Optical experiments on the SWNT fractions revealed that the…
We studied optical absorption of single-walled carbon nanotubes by varying the dielectric environment. For the two different components of the broad UV absorption feature conventionally referred to as the pi-plasmon, we find that the component at 5.0 - 5.3 eV exhibits remarkable spectral changes, based on which we attribute this to a dipolar radial surface plasmon. However, the component at ~4.5 eV remains unchanged, raising a fundamental question as to its conventional attribution. We discuss its relation with the absorption feature at ~4.5 eV in graphite arising from an interband transition.
The influence of carbon multi-walled nanotubes (MWCNTs) and halloysite nanotubes (HNTs) on the physical, thermal, mechanical, and electrical properties of EVA (ethylene vinyl acetate) copolymer was investigated. EVA-based nanocomposites containing MWCNTs or HNTs, as well as hybrid nanocomposites containing both nanofillers were prepared by melt blending. Scanning electron microcopy (SEM) images revealed the presence of good dispersion of both kinds of nanotubes throughout the EVA matrix. The incorporation of nanotubes into the EVA copolymer matrix did not significantly affect the crystallizati…
Having access to the chemical environment at the atomic level of a dopant in a nanostructure is crucial for the understanding of its properties. We have performed atomically-resolved electron energy-loss spectroscopy to detect individual nitrogen dopants in single-walled carbon nanotubes and compared with first principles calculations. We demonstrate that nitrogen doping occurs as single atoms in different bonding configurations: graphitic-like and pyrrolic-like substitutional nitrogen neighbouring local lattice distortion such as Stone-Thrower-Wales defects. The stability under the electron b…
Combining a classical force field, a tight-binding model, and first-principles calculations, we have studied structural, electronic, and optical properties of double-walled carbon nanotube (DWNT) bundles under hydrostatic pressure. We find that the outer tube acts as a protection shield for the inner tube and the inner tube increases the structure stability and the ability to resist the pressure of the outer tube. Moreover, the collapsed structures of the double-walled carbon nanotube bundle called ``parallel'' and ``in-between'' are more stable than the one called ``herringbone''. The structu…
The elasticity and piezoelectricity of zinc oxide (ZnO) crystals and single layers are investigated from the first-principles calculations. It is found that a ZnO thin film less than three Zn-O layers prefers a planar graphite-like structure to the wurtzite structure. ZnO single layers are much more flexible than graphite single layers in the elasticity and stronger than boron nitride single layers in the piezoelectricity. Single-walled ZnO nanotubes (SWZONTs) can exist in principle because of their negative binding energy. The piezoelectricity of SWZONTs depends on their chirality. For most Z…
A first-principles investigation of the electronic and quantum transport properties of double-walled carbon nanotubes doped with nitrogen and boron atoms is presented. Concentric nanotube sidewalls separated by the typical graphitic van der Waals bond distance are found to strongly interact upon incorporation of doping atoms in the hexagonal networks. The local perturbation caused by the doping atoms extends over both shells due to a hybridization of their electronic states, yielding a reduction of the backscattering efficiency as compared with two independent single-walled nanotubes. A multi-…
Single air-suspended carbon nanotubes (length 2 - 5 microns) exhibit high optical quantum efficiency (7 - 20%) for resonant pumping at low intensities. Under ultrafast excitation, the photoluminescence dramatically saturates for very low injected exciton numbers (2 to 6 excitons per pulse per SWCNT). This PL clamping is attributed to highly efficient exciton-exciton annihilation over micron length scales. Stochastic modeling of exciton dynamics and femtosecond excitation correlation spectroscopy allow determination of nanotube absorption (2 - 6%) and exciton lifetime (85 +- 20 ps).
Cross-polarized absorption peaks of isolated single-walled carbon nanotubes were observed by a polarized photoluminescence excitation (PLE) spectroscopy. Using a simple theory for PL anisotropy, the observed PLE spectra are decomposed into 'pure' components of the photoexcitation for incident light polarized parallel and perpendicular to the SWNT axis. For several (n, m) SWNTs, distinct peaks corresponding to perpendicular excitation were observed. The measured transition energies for perpendicular excitations were blue-shifted compared to the qualitative values predicted within a single-parti…
Single-walled carbon nanotubes are hollow cylinders, that can grow centimeters long by carbon incorporation at the interface with a catalyst. They display semi-conducting or metallic characteristics, depending on their helicity, that is determined during their growth. To support the quest for a selective synthesis, we develop a thermodynamic model, that relates the tube-catalyst interfacial energies, temperature, and the resulting tube chirality. We show that nanotubes can grow chiral because of the configurational entropy of their nanometer-sized edge, thus explaining experimentally observed …
Single-walled carbon nanotubes (SWCNTs) are quasi-one-dimensional systems with poor Coulomb screening and enhanced electron-phonon interaction, and are good candidates for excitons and exciton-phonon couplings in metallic state. Here we report back scattering reflection experiments on individual metallic SWCNTs. An exciton-phonon sideband separated by 0.19 eV from the first optical transition peak is observed in a metallic SWCNT of chiral index (13,10), which provides clear evidences of excitons in metallic SWCNTs. A static dielectric constant of 10 is estimated from the reflectance spectrum.
The electronic breakdown and the bias dependence of the conductance have been investigated for a large number of catalytic chemical vapor deposition (CCVD) grown single-walled carbon nanotubes (SWCNTs) with very small diameters. The convenient fabrication of thousands of properly contacted SWCNTs was possible by growth on electrode structures and subsequent electroless palladium deposition. Almost all of the measured SWCNTs showed at least weak gate dependence at room temperature. Large differences in the conductance and breakdown behavior have been found for "normal" semiconducting SWCNTs and…
Symmetric minima of surface potential energy of a nanocatalyst act as nucleation sites for chirally selective initial growth of single walled carbon tubes at low temperatures. The nucleation sites are sites of maximum coordination number of the adsorbed carbon. We show this using the five fold symmetry of a pentagonal pyramid of an icosahedron. Initial zigzag structure from nucleation sites results in formation of hexagons and pentagons that result in anomalous cap formation. Possible cap lift off mechanism is discussed.
Structural identification of double-walled carbon nanotubes (DWNT) is presented through a robust procedure based on the latest generation of transmission electron microscope, making possible a statistical analysis based on numerous nano-objects. This approach reveals that inner and outer tubes of DWNTs are not randomly oriented, suggesting the existence of a mechanical coupling between the two concentric walls. With the support of atomic scale modelisations, we attribute it to the presence of incommensurate domains whose structures depend on the diameters and helicities of both tubes, and wher…
Three kinds of the response mechanisms to the external pressure have been found for double-walled carbon nanotube (DWNT) bundle, depending strongly on their average radius and symmetry. The small-diameter DWNT bundle undergoes a small discontinuous volume change, and then deform continuously. The intermediate-diameter DWNT bundle collapses completely after a structure phase transition (SPT). Significantly, two SPTs exist for the larger-diameter DWNT bundle if the outer tube has no $C_{6}$ or $C_{3}$ symmetry. It would be interesting to search for signatures of these different structural transf…
The results of a study on the evolution of HiPco single-walled carbon nanotubes during the oxidizing action of H2SO4 and HNO3 are presented. The process conditions used have been chosen so as to avoid any significant damage to the nanotube structure. The type and level of functionalization, the location of the grafted functions on the surface of the nanotube and the changes in morphological characteristics of the samples were examined by using a wide and complementary range of analytical techniques. We propose an explanation for the differences in the oxidizing action of sulfuric and nitric ac…
Exposing single-walled carbon nanotubes to room temperature UV-generated ozone leads to an irreversible increase in their electrical resistance. We demonstrate that the increased resistance is due to ozone oxidation on the sidewalls of the nanotubes rather than at the end caps. Raman and x-ray photoelectron spectroscopy show an increase in the defect density due to the oxidation of the nanotubes. Using ultraviolet photoelectron spectroscopy we show that these defects represent the removal of pi-conjugated electron states near the Fermi level, leading to the observed increase in electrical resi…
We theoretically investigate the impact of the electrothermal flow on the dielectrophoretic separation of single-walled carbon nanotubes (SWNT). The electrothermal flow is observed to control the motions of semiconducting SWNTs in a sizeable domain near the electrodes under typical experimental conditions, therefore helping the dielectrophoretic force to attract semiconducting SWNTs in a broader range. Moreover, with the increase of the surfactant concentration, the electrothermal flow is enhanced, and with the change of frequency, the pattern of the electrothermal flow changes. It is shown th…
An elongation method based on ab initio quantum chemistry approaches is presented. It allows to study electronic structures and coherent electron transportation properties of single-walled carbon nanotubes (SWCNTs) up to 22nm in length using the hybrid density functional theory. The 22nm long SWCNT, consisting of more than ten thousands electrons, is the largest carbon nanotube that has ever been studied at such a sophisticated all-electron level. Interesting oscillating behaviour of the energy gap with respect to the length of the nanotube is revealed. The calculated current-voltage character…
In this work, phosphorous-doped single-walled carbon nanotubes have been synthesized by the thermal decomposition of trimethylphosphine using a high-vacuum chemical vapor deposition method. Furthermore, a modified density-gradient-ultracentrifugation process has been applied to carefully purify our doped material. The combined use of Raman and X-ray photoelectron spectroscopy allowed us to provide the first insight into the bonding environment of P incorporated into the carbon lattice, avoiding competing signals arising from synthesis byproducts. This study represents the first step toward the…
The structural, electronic, optical and vibrational properties of the collapsed (10,10) single-walled carbon nanotube bundle under hydrostatic pressure have been studied by the first-principles calculations. Some features are observed in the present study: First, a collapsed structure is found, which is distinct from both of the herringbone and parallel structures obtained previously. Secondly, a pseudo-gap induced by the collapse appears along the symmetry axis \textit{$Γ$X}. Thirdly, the relative orientation between the collapsed tubes has an important effect on their electronic, optical and…
Carbon nanotubes are a good realization of one-dimensional crystals where basic science and potential nanodevice applications merge. Defects are known to modify the electrical resistance of carbon nanotubes. They can be present in as-grown carbon nanotubes, but controlling externally their density opens a path towards the tuning of the nanotube electronic characteristics. In this work consecutive Ar+ irradiation doses are applied to single-walled nanotubes (SWNTs) producing a uniform density of defects. After each dose, the room temperature resistance versus SWNT-length [R(L)] along the nanotu…
The present communication highlights that ac conductivity measurement of the multi-walled carbon nanotubes (MWNTs)-polymer composites is a very promising characterizing tool for qualifying any crude MWNT-sample synthesized by electric arc. It distinguishes graphite structures from that of the MWNTs and reflects the relative amount of nearly one-dimensional structures and disorders present within the samples. This new protocol would help in evolving more direct and quantitative criteria for qualification of MWNTs synthesized through diverse techniques and will definitely add up to the conceptua…
The stabilization of carbon nanotubes via the filling with inner tubes is demonstrated by probing the optical transitions in double-walled carbon nanotube bundles under hydrostatic pressure with optical spectroscopy. Double-walled carbon nanotube films were prepared from fullerene peapods and characterized by HRTEM and optical spectroscopy. In comparison to single-walled carbon nanotubes, the pressure-induced redshifts of the optical transitions in the outer tubes are significantly smaller below $\sim$10 GPa, demonstrating the enhanced mechanical stability due to the inner tube already at low …
The radial-breathing-like phonon modes (RBLMs) of the double-walled carbon nanotubes are studied in a simple analytical model, in which the interaction force constants (FCs) can be obtained analytically from the continuous model. The RBLMs frequencies are obtained by solving the dynamical matrix, and their relationship with the tube radii can be obtained analytically, offering a powerful experimental tool for determining precisely the radii of the multi-walled carbon nanotubes.
Based on the van der Waals interaction, the periodically nonlinear potential of a singe-walled carbon nanotube (SWNT) with finite length in an infinite length SWNT is analytically obtained. It is found that the inner SWNT can oscillate in the outer SWNT with frequency beyond ten Gigahertz, even up to a hundred Gigahertz.
Semiconducting single-walled carbon nanotubes are studied in the diffusive transport regime. The peak mobility is found to scale with the square of the nanotube diameter and inversely with temperature. The maximum conductance, corrected for the contacts, is linear in the diameter and inverse temperature. These results are in good agreement with theoretical predictions for acoustic phonon scattering in combination with the unusual band structure of nanotubes. These measurements set the upper bound for the performance of nanotube transistors operating in the diffusive regime.
Towards the development of a useful mechanism for hydrogen storage, we have studied the hydrogenation of single-walled carbon nanotubes with atomic hydrogen using core-level photoelectron spectroscopy and x-ray absorption spectroscopy. We find that atomic hydrogen creates C-H bonds with the carbon atoms in the nanotube walls and such C-H bonds can be com-pletely broken by heating to 600 oC. We demonstrate approximately 65+/-15 at % hydrogenation of carbon atoms in the single-walled carbon nanotubes which is equivalent to 5.1+/-1.2 weight % hydrogen capacity. We also show that the hydrogenation…
