Experiments with irradiated single-walled carbon nanotubes are shown to generate a set of probability distribution functions and to derive a set of information theoretic entropy-based parameters. Energetic Cs+ ions initiate linear collision cascades and nonlinear thermal spikes in single-walled carbon nanotubes. The probability distribution functions are constructed from the normalized experimental yields of the sputtered atoms and clusters. The information or Shannon entropy and fractal dimension are evaluated for each of the emitted species. Along with the fractal dimension, the information is used to identify and distinguish the energy dissipation processes that generate conditions for monatomic sputtering and clusters emissions.
Direct measurements of the diffusion length of excitons in air-suspended single-walled carbon nanotubes are reported. Photoluminescence microscopy is used to identify individual nanotubes and to determine their lengths and chiral indices. Exciton diffusion length is obtained by comparing the dependence of photoluminescence intensity on the nanotube length to numerical solutions of diffusion equations. We find that the diffusion length in these clean, as-grown nanotubes is significantly longer than those reported for micelle-encapsulated nanotubes.
We investigate the energy spectra of clean incommensurate double-walled carbon nanotubes, and find that the overall spectral properties are described by the so-called critical statistics of Anderson metal-insulator transition. In the energy spectra, there exist three different regimes characterized by Wigner-Dyson, Poisson, and semi-Poisson distributions. This feature implies that the electron transport in incommensurate multi-walled nanotubes can be either diffusive, ballistic, or intermediate between them, depending on the position of the Fermi energy.
We have contacted single-walled carbon nanotubes after aligning the tubes by the use of surface acoustic waves. The acoustoelectric current has been measured at 4.2 K and a probing of the low-dimensional electronic states by the surface acoustic wave has been detected. By decreasing the acoustic wavelength resulting in an adjustment to the length of the defined carbon nanotube constriction a quantization of the acoustoelectric current has been observed.
We report experimental measurements of electronic Raman scattering under resonant conditions by electrons in individual single-walled carbon nanotubes (SWNTs). The inelastic Raman scattering at low frequency range reveals a single particle excitation feature and the dispersion of electronic structure around the center of Brillouin zone of a semiconducting SWNT (14, 13) is extracted.
Relatively low magnetic fields applied parallel to the axis of a chiral single-walled carbon nanotube are found causing large modulations to the p-channel or valence band conductance of the nanotube in the Fabry-Perot interference regime. Beating in the Aharonov-Bohm type of interference between two field-induced non-degenerate sub-bands of spiraling electrons is responsible for the observed modulation with a pseudo period much smaller than that needed to reach the flux quantum F0 = h/e through the nanotube cross-section. We show that single-walled nanotubes represent the smallest cylinders ex…
We investigate the propagation of electron wavepackets in single-walled carbon nanotubes via a Lindblad-based density-matrix approach that enables us to account for both dissipation and decoherence effects induced by various phonon modes. We show that, while in semiconducting nanotubes the wavepacket experiences the typical dispersion of conventional materials, in metallic nanotubes its shape remains essentially unaltered, even in the presence of the electron-phonon coupling, up to micron distances at room temperature.
We investigate electronic transport properties of Schottky-barrier field-effect transistors (FET) based on double-walled carbon nanotubes (DWNT) with a semiconducting outer shell and a metallic inner one. These kind of DWNT-FET show asymmetries of the $I$-$V$ characteristics and threshold voltages due to the electron-hole asymmetry of the Schottky barrier. The presence of the metallic inner shell induces a large effective band gap, which is one order of magnitude larger than that due to the semiconducting shell alone of a single-walled carbon nanotube FET.
We characterized the energy band dispersion near the Fermi level in single-walled carbon nanotubes using low-temperature scanning tunneling microscopy. Analysis of energy dependent standing wave oscillations, which result from quantum interference of electrons resonantly scattered by defects, yield a linear energy dispersion near EF, and indicate the importance of parity in scattering for armchair single-walled carbon nanotubes. Additionally, these data provide values of the tight-binding overlap integral and Fermi wavevector in good agreement with previous work, but indicate that the electron…
Single walled carbon nanotube's cross section can be flattened under hydrostatic pressure. One example is the cross section of a single walled carbon nanotube successively deforms from the original round shape to oval shape, then to peanut-like shape. At the transition point of reversible deformation between convex shape and concave shape, the side wall of nanotube is flattest. This flattest tube has many attractive properties. In the present work, an approximate approach is developed to determine the equilibrium shape of this unstrained flattest tube and the curvature distribution of this tub…
A variational solution of the coupled electron-phonon Boltzmann equations is used to calculate the phonon drag contribution to the thermopower in a 1-D system. A simple formula is derived for the temperature dependence of the phonon drag in metallic, single-walled carbon nanotubes. Scattering between different electronic bands yields nonzero values for the phonon drag as the Fermi level varies.
We identify a new material phenomenon, where minute mechanical manipulations induce pronounced global structural reconfigurations in faceted multi-walled nanotubes. This behavior has strong implications on the tribological properties of these systems and may be the key to understand the enhanced inter-wall friction recently measured for boron-nitride nanotubes with respect to their carbon counterparts. Notably, the fast rotation of helical facets in these systems upon coaxial sliding may serve as a nanoscale Archimedean screw for directional transport of physisorbed molecules.
We propose a simple approach to construct a quantum-dot and it's electrodes using chiral metallic single walled carbon nanotube (CM-SWCNT) segments of exactly opposite chiralities $(m,n)$ and $(n,m)$. The degree and energetics of electron confinement crucially depends on the choice of $n$ and $m$, and collinearity of the SWCNT segments constituting the quantum-dot and the electrodes. All the segments can in principle be obtained through simple manipulations of fragments of a single nanotube of chirality either $(m,n)$ or $(n,m)$.
We report the experimental realization of double quantum dots in single-walled carbon nanotubes. The device consists of a nanotube with source and drain contact, and three additional top-gate electrodes in between. We show that, by energizing these top-gates, it is possible to locally gate a nanotube, to create a barrier, or to tune the chemical potential of a part of the nanotube. At low temperatures we find (for three different devices) that in certain ranges of top-gate voltages our device acts as a double quantum dot, evidenced by the typical honeycomb charge stability pattern.
Electrical transport through single-walled carbon nanotubes (SWNTs) is investigated by using the nearest-neighbor tight-binding model coupled with two electron reservoirs. When the SWNT-electrode coupling is not axially symmetric, asymmetric resonance peaks are found in the conductance and are considered to be due to the interference between two transport channels. These Fano resonances are sensitive to the coupling with electrodes. When the coupling is axially symmetric, no asymmetric resonance peaks are observed.
We demonstrate a fully tunable diode structure utilizing a fully suspended single-walled carbon nanotube (SWNT). The diode's turn-on voltage under forward bias can be continuously tuned up to 4.3 V by controlling gate voltages, which is ~6 times the nanotube bandgap energy. Furthermore, the same device design can be configured into a backward diode by tuning the band-to-band tunneling current with gate voltages. A nanotube backward diode is demonstrated for the first time with nonlinearity exceeding the ideal diode. These results suggest that a tunable nanotube diode can be a unique building b…
AFM manipulation was used to controllably stretch individual metallic single-walled carbon nanotubes (SWNTs). We have found that SWNTs can sustain elongations as great as 30% without breaking. Scanned gate microscopy and transport measurements were used to probe the effects of the mechanical strain on the SWNT electronic properties, which revealed a strain-induced increase in intra-tube electronic scattering above a threshold strain of ~5-10%. These findings are consistent with theoretical calculations predicting the onset of plastic deformation and defect formation in carbon nanotubes.
The recently reported experimental optical spectra of double-walled carbon nanotubes exhibit more peaks than it could be expected based on the layers alone. The appearance of excess peaks has been attributed to the interlayer interaction. In order to elucidate the origin of the excess peaks, we perform calculations of the optical absorption of a particular nanotube using the recursion method with non-orthogonal tight-binding basis functions. Our study shows that the interlayer interaction can give rise to major changes in the electronic structure of this nanotube, manifesting themselves with s…
A correlation is observed between the diameter (d) distribution of single walled carbon nanotubes and the percentages of metallic and semiconducting tubes in materials synthesized at low temperature (600 C) by plasma-assisted chemical vapor deposition. Small diameter nanotubes (average d~1.1 nm) show semiconducting-tube percentage much higher than expected for random chirality distribution. Density functional theory calculations reveal discernable differences in the cohesive energies and heat of formation energies for similar-diameter metallic, quasi-metallic and semiconducting nanotubes. Semi…
Gate-voltage effects on photoluminescence spectra of suspended single-walled carbon nanotubes are investigated. Photoluminescence microscopy and excitation spectroscopy are used to identify individual nanotubes and to determine their chiralities. Under an application of gate voltage, we observe slight blueshifts in the emission energy and strong quenching of photoluminescence. The blueshifts are similar for different chiralities investigated, suggesting extrinsic mechanisms. In addition, we find that the photoluminescence intensity quenches exponentially with gate voltage.
Recent measurements in single-walled carbon nanotubes show that, on resonance, all nanotubes display the same peak optical conductivity of approximately 8 $e^2/h$, independent of radius or chirality [Joh \emph{et al.}, \emph{Nature Nanotechnology} \textbf{6}, 51 (2011)]. We show that this uniform peak conductivity is a consequence of the relativistic band structure and strength of the Coulomb interaction in carbon nanotubes. We further construct a minimalist model of exciton dynamics that describes the general phenomenology and provides an accurate prediction of the numerical value of the peak…
We report the capacitive spring softening effect observed in single-walled carbon nanotube (SWNT) nanoelectromechanical (NEM) resonators. The nanotube resonators adopt dual-gate configuration with both bottom-gate and side-gate capable of tuning the resonance frequency through capacitive coupling. Interestingly, downward resonance frequency shifting is observed with increasing side-gate voltage, which can be attributed to the capacitive softening of spring constant. Furthermore, in-plane vibrational modes exhibit much stronger spring softening effect than out-of-plan modes. Our dual-gate desig…
Centimeter scale aligned carbon nanotube arrays are grown from nanoparticle metal catalyst pads. We find the nanotubes grow both with and against the wind. A metal underlayer provides in-situ electrical contact to these long nanotubes with no post growth processing needed. Using the electrically contacted nanotubes, we study electrical transport of 0.4 cm long nanotubes. The source drain I-V curves are quantitatively described by a classical, diffusive model. Our measurements show that the outstanding transport properties of nanotubes can be extended to the cm scale and open the door to large …
We report optically induced aggregation and consequent separation of specific diameter of pristine single walled carbon nanotubes (SWNT) from stable solution. Well dispersed solution of pristine SWNTs, without any surfactant or functionalization, show rapid aggregation by uniform exposure to UV, visible and NIR illumination. Optically induced aggregation linearly increases with consequent increase in the intensity of light. Aggregated SWNTs were separated from the dispersed supernatant and characterized using absorption and Raman spectroscopy. Separated SWNTs distinctly show enrichment of spec…
The interactions between the layers of double-walled carbon nanotubes induce measurable shift of the G bands relative to the isolated layers. While experimental data on this shift in free-standing double-walled carbon nanotubes has been reported in the past several years, comprehensive theoretical description of the observed shift is still lacking. The prediction of this shift is important for supporting the assignment of the measured double-walled nanotubes to particular nanotube types. Here, we report a computational study of the G-band shift as a function of the semiconducting inner layer r…
We characterize the energy loss of the non-equilibrium electron system in individual metallic single-walled carbon nanotubes at low temperature. Using Johnson noise thermometry, we demonstrate that, for a nanotube with ohmic contacts, the dc resistance at finite bias current directly reflects the average electron temperature. This enables a straightforward determination of the thermal conductance associated with cooling of the nanotube electron system. In analyzing the temperature- and length-dependence of the thermal conductance, we consider contributions from acoustic phonon emission, optica…
We study the low frequency current correlations of an individual single-walled carbon nanotube at liquid He temperature. We have distinguished two physical regimes -- zero dimensional quantum dot and one dimensional quantum wire -- in terms of an energy spacing from the finite tube length in both differential conductance and shot noise measurements. In a one dimensional wire regime, we observed a highly suppressed shot noise from all measured tube devices, suggesting that electron-electron interactions play an important role.
Non-dispersive, inter-layer interaction induced Raman peaks (I bands) -- in the region of the D band -- have been observed recently for bilayer graphene, when the two layers were rotated with respect to each other. Here, similar observations for double-walled carbon nanotubes (DWCNTs) are theoretically predicted. The prediction is based on double resonance theory, involving non-zone-centered phonons, and the effect of disorder is replaced by interaction between the two tubes.
The role of self-heating and hot-phonons on electronic transport in metallic single walled carbon nanotube is examined by solving a coupled electron-optical phonon (OP) Boltzmann transport equation and the classical heat equation. We find that self-heating reduces the high bias conductance, thus explaining the short OP mean free paths observed experimentally, while the non-equilibrium OP population reduces the overall current level. Comparison with experimental data shows that for tubes on a substrate, no significant population of hot phonons builds up under the normal range of applied bias. T…
The temperature distributions in current-carrying carbon nanotubes have been measured with a scanning thermal microscope. The obtained temperature profiles reveal diffusive and dissipative electron transport in multi-walled nanotubes and in single-walled nanotubes when the voltage bias was higher than the 0.1-0.2 eV optical phonon energy. Over ninety percent of the Joule heat in a multi-walled nanotube was found to be conducted along the nanotube to the two metal contacts. In comparison, about eighty percent of the Joule heat was transferred directly across the nanotube-substrate interface for…
The fabrication of metallic single-walled carbon nanotube electrodes separated by gaps of typically 20nm width by electron-beam-induced oxidation is studied within an active device configuration. The tube conductance is measured continuously during the process. The experiment provides a statistical evaluation of gap sizes as well as the electron dose needed for gap formation. Also, the ability to precisely cut many carbon nanotubes in parallel is demonstrated.
We report electrical transport experiments using the phenomenon of electrical breakdown to perform thermometry that probe the thermal properties of individual multi-walled nanotubes. Our results show that nanotubes can readily conduct heat by ballistic phonon propagation, reaching a quantum-mechanical limit to thermal conductance. We determine the thermal conductance quantum, the ultimate limit to thermal conductance for a single phonon channel, and find good agreement with theoretical calculations. Moreover, our results suggest a breakdown mechanism of thermally activated C-C bond breaking co…
We report experimental observation of impedance oscillations in single-walled carbon nanotubes measured from 100 MHz to 65 GHz on coplanar wave guides and a power law dependence of the differential conductance with bias voltage. From the crossover of the real and imaginary parts of the complex impedance observed in the range of 10 GHz, we estimate a long lifetime of 15 ps that can support the claim of ballistic transport. By measuring the scattering parameters at high-frequencies of a few aligned single-walled bundles at low temperatures we show that, this observation is strongly influenced by…
The low quality factor (Q) of Single-walled carbon nanotube (SWNT) resonators has limited their sensitivity in sensing application. To this end, we employ the technique of parametric amplification by modulating the spring constant of SWNT resonators at twice the resonant frequency, and achieve 10 times Q enhancement. The highest Q obtained at room temperature is around ~700, which is 3-4 times better than previous Q record reported for doubly-clamped SWNT resonators. Furthermore, efficient parametric amplification is found to only occur in the catenary vibration regime. Our results open up the…
We characterize the terahertz detection mechanism in antenna-coupled metallic single-walled carbon nanotubes. At low temperature, 4.2 K, a peak in the low-frequency differential resistance is observed at zero bias current due to non-Ohmic contacts. This electrical contact nonlinearity gives rise to the measured terahertz response. By modeling each nanotube contact as a nonlinear resistor in parallel with a capacitor, we determine an upper bound for the value of the contact capacitance that is smaller than previous experimental estimates. The small magnitude of this contact capacitance has favo…
In a telescoped double-walled nanotube (TDWNT), with the inner tube partially extracted from the outer tube, the total current is forced to flow between the layers. Considering the interlayer Hamiltonian as a perturbation, we can obtain an analytic formula for the interlayer conductance. The accuracy of the perturbation formula is systematically improved by including higher-order terms. The interlayer interaction effective in the perturbation formula is the product of the interlayer Hamiltonian and the wave function. It clarifies the effects of the spatial range of the interlayer Hamiltonian a…
We report a combined electronic transport and structural characterization study of small carbon nanotube bundles in field-effect transistors (FET). The atomic structures of the bundles are determined by electron diffraction using an observation window built in the FET. The single-walled nanotube bundles exhibit electrical transport characteristics sensitively dependent on the structure of individual tubes, their arrangements in the bundle, deformation due to intertube interaction, and the orientation with respect to the gate electric field. Our ab-initio simulation shows that tube deformation …
We have measured shot noise in single walled carbon nanotubes (SWNT) with good contacts at 4.2 K at low frequencies ($f=600 - 850$ MHz). We find a strong modulation of shot noise over the Fabry-Perot pattern; in terms of differential Fano factor the variation ranges over 0.4 - 1.2. The shot noise variation, in combination with differential conductance, is analyzed using two (spin-degenerate) modes with different, energy-dependent transmission coefficients. No power law dependence of shot noise, as expected for Luttinger liquids, was found in our measurements.
We calculate the current-voltage characteristic of a homogeneously strained metallic carbon nanotube adsorbed on a substrate. The strain generates a gap in the energy spectrum leading to a reduction of the current. In the elastic regime, the current-voltage characteristic shows a large negative differential conductance at bias voltages of around $ \gtrsim 0.17 $V. We discuss the implications for the current in the superelongated regime.
We are proposing a novel method of laser heating control only through change in polarization of the incident light, keeping its power density constant. The idea combines antenna effect found in isolated multi-walled carbon nanotubes and the possibility of their heating by light illumination. To observe this we used Raman spectroscopy technique, where the heating manifests itself in a pronounced downshift of the Raman G and 2D lines as a function of the polarization angle. Our method can be useful in field electron emission devices or in selective nanotubes heating and destruction. It can also …
We have performed transport spectroscopy on individual ropes of single-walled carbon nanotubes. We find that the levels are Zeeman split in a magnetic field, with a g-factor of 2.04 +- 0.05. The observed pattern of peak splittings indicates the parity of the number of electrons on the dot. In one device there are also signs of the presence of a second dot. We observe features which resemble anticrossings between quantum levels in the two dots, which may be formed from separate conducting nanotubes within the rope.
We study the electrical transport properties of well-contacted ballistic single-walled carbon nanotubes in a three-terminal configuration at low temperatures. We observe signatures of strong electron-electron interactions: the conductance exhibits bias-voltage-dependent amplitudes of quantum interference oscillation, and both the current noise and Fano factor manifest bias-voltage-dependent power-law scalings. We analyze our data within the Tomonaga-Luttinger liquid model using the non-equilibrium Keldysh formalism and find qualitative and quantitative agreement between experiment and theory.
We explore the nature of anomalous diffusion of wave packets in disorder-free incommensurate multi-walled carbon nanotubes. The spectrum-averaged diffusion exponent is obtained by calculating the multifractal dimension of the energy spectrum. Depending on the shell chirality, the exponent is found to lie within the range $1/2 \leq η< 1$. For large unit cell mismatch between incommensurate shells, $η$ approaches the value 1/2 for diffusive motion. The energy-dependent quantum spreading reveals a complex density-of-states-dependent pattern with ballistic, super-diffusive or diffusive character.
We show that a multi-walled carbon nanotube film can be used as the sensing element of a low-cost sensor for the alcoholic concentration in liquid solutions. To this purpose, we investigate the electrical resistance of the film as a function of the isopropanol concentration in a water solution. The analysis reveals a growing resistance with increasing isopropanol concentration and a fast response. The sensing element is re-usable as the initial resistance value is restored once the solution has evaporated. The electrical resistance increases linearly when the multi-walled carbon nanotube film …
We used scattering-type scanning near-field optical microscopy (s-SNOM) to characterize nickel nanoclusters grown inside single-walled carbon nanotubes (SWCNT). The nanotubes were filled with Ni(II) acetylacetonate and the molecules were transformed into nickel clusters via annealing. The metal clusters give high local contrast enhancement in near-field phase maps caused by the excitation of free charge carriers. The near-field contrast was simulated using the finite dipole model, approximating the clusters with elliptical nanoparticles. Compared to magnetic force microscopy, s-SNOM appears mu…
Single electron transistors (SETs) are fabricated by placing single walled carbon nanotubes (SWNTs) on a 100 nm wide local Al/Al2O3 bottom gate and then contacting with Pd electrodes. Coulomb oscillations up to 125 K were observed and charging energies of 12-15 meV with level spacing of ~5 meV were measured from the Couloumb diamond, in agreement with a dot size of ~100 nm, implying that the local gate defines the dot size by bending SWNT at the edges and controls its operation. This "mechanical template" approach may facilitate large scale fabrication of SET devices using SWNT.
We have studied photocurrent generation in large carbon nanotube (CNT) films using electrodes with different spacings. We observe that the photocurrent depends strongly on the position of illumination, with maximum observed response occurring upon illumination at the electrode edges. The rate of change of the response decays exponentially, with the fastest response occurring for samples with the smallest electrode spacing. We show that the time response is due to charge carrier diffusion in low-mobility CNT films.
The transport properties of quantum dot (QD) systems based on double-walled carbon nanotube (DWCNT) are investigated. The interplay between microscopic structure and strong Coulomb interaction is treated within a bosonization framework. The linear and nonlinear G-V-V_g characteristics of the QD system is calculated by starting from the Liouville equation for the reduced density matrix. Depending on the intershell couplings, an 8-electron periodicity of the Coulomb blockade peak spacing in the case of commensurate DWCNT QDs and a 4-electron periodicity in the incommensurate case are predicted. …
We characterize radio frequency detection in a high-quality metallic single-walled carbon nanotube. At a bath temperature of 77 K, only bolometric (thermal) detection is seen. At a bath temperature of 4.2 K and low bias current, the response is due instead to the electrical nonlinearity of the non-ohmic contacts. At higher bias currents, the contacts recover ohmic behavior and the observed response agrees well with the calculated bolometric responsivity. The bolometric response is expected to operate at terahertz frequencies, and we discuss some of the practical issues associated with developi…
We present the results of analytical study and Molecular Dynamics simulation of low energy nonlinear non-stationary dynamics of single-walled carbon nanotubes (CNTs). New phenomena of intensive energy exchange between different parts of CNT and weak energy localization in a part CNT are analytically predicted in the framework of the continuum shell theory. These phenomena take place for CNTs of finite length with medium aspect ratio under different boundary conditions. Their origin is clarified by means of the concept of Limiting Phase Trajectory, and the analytical results are confirmed by th…
We report measurements on ropes of Single Walled Carbon Nanotubes (SWNT) in low-resistance contact to non-superconducting (normal) metallic pads, at low voltage and at temperatures down to 70 mK. In one sample, we find a two order of magnitude resistance drop below 0.55 K, which is destroyed by a magnetic field of the order of 1T, or by a d.c. current greater than 2.5 microA. These features strongly suggest the existence of superconductivity in ropes of SWNT.
Single walled carbon nanotubes of 2 nm diameter and 3 to 13 micro meter length were compressed in Cu bullets and irradiated with positive ions of Cs with energies from 0.2 to 2.0 keV and subjected to successively increasing Cs dose. From the mass spectra of the sputtered carbon atoms and clusters as a function of Cs energy the monitoring of trend of the relative number densities of the fragmenting species indicates the accumulating damage. Irradiation induced fragmentation provide clues to the structural changes as a result of creation of vacancies due to the sputtering of monatomic, diatomic,…
The structure and elastic properties of (5,5) and (10,10) nanotubes, as well as barriers for relative rotation of the walls and their relative sliding along the axis in a double-walled (5,5)@(10,10) carbon nanotube, are calculated using the density functional method. The results of these calculations are the basis for estimating the following physical quantities: shear strengths and diffusion coefficients for relative sliding along the axis and rotation of the walls, as well as frequencies of relative rotational and translational oscillations of the walls. The commensurability-incommensurabili…
We present evidence of all optical trion generation and emission in undoped single walled carbon nanotubes (SWCNTs). Luminescence spectra, recorded on individual SWCNTs over a large CW excitation intensity range, show trion emission peaks red-shifted with respect to the bright exciton peak. Clear chirality dependence is observed for 22 separate SWCNT species, allowing for determination of electron-hole exchange interaction and trion binding energy contributions. Luminescence data together with ultrafast pump probe experiments on chirality sorted bulk samples suggest that exciton-exciton annihi…
Experimental results from irradiated-carbon nanostructures can be partially explained by selective applications of classical damage theories and ad-hoc thermal models by treating the binary atomic collision cascades and multi-atomic thermal spikes as energy-dissipating mechanisms. An information-theoretic model is developed by treating the irradiated single-walled carbon nanotubes and C60 as entropy-generating dissipative structures. The model is based on evaluating the experimental probability distribution functions of the sputtered constituents and components from the irradiated carbon nanos…
We report the first high-field magneto-optical study on the exciton-phonon sideband of single-walled carbon nanotubes (SWNTs) consisting only of (6,5) species. Both energy and intensity of the observed phonon sideband were found to be independent of the external magnetic field. Comparing with theoretical calculations, we confirmed that these sidebands originate from the optically forbidden K-momentum singlet excitons. Energy of these K-momentum dark excitons was extracted to be ~ 21.5 meV above the bright zero-momentum singlet excitons, in close agreement with recent theoretical predictions an…
We show that optical second-harmonic generation (SHG) can be observed from individual single-walled carbon nanotubes (SWCNTs) and, furthermore, allows imaging of individual tubes. Detailed analysis of our results suggests that the structural noncentrosymmetry, as required for SHG, arises from the non-zero chiral angle of the SWCNT. SHG thus has potential as a fast, non-destructive, and simple method for imaging of individual nanomolecules and for probing their chiral properties. Even more, it opens the possibility to optically determine the handedness of individual SWCNTs.
We report a computational study, using the "moments method" [Y. Gao and M. Daw, Modelling Simul. Mater. Sci. Eng. 23 045002 (2015)], of the anharmonicity of the vibrational modes of single-walled carbon nanotubes. We find that modes with displacements largely within the wall are more anharmonic than modes with dominantly radial character, except for a set of modes that are related to the radial breathing mode which are the most anharmonic of all. We also find that periodicity of the calculation along the tube length does not strongly affect the anharmonicity of the modes, but that the tubes wi…
Auger-ionized carriers in a one-dimensional semiconductor are predicted to result in a strong band-gap renormalization. Isolated single-walled carbon nanotubes (SWCNT) under high-intensity laser irradiation exhibit strong nonlinear photoluminescence (PL) due to exciton-exciton annihilation (EEA). The presence of exciton disassociation during the rapid Auger-ionization caused by EEA would lead to a strong nonlinear absorption. By simultaneously measuring SWCNT PL and optical absorption of isolated SWCNT clusters in the PL saturation regime, we give evidence that Auger-ionized excitons do not di…
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.
