To optimize the performance of multifunctional carbon nanotube-ferroelectric devices, it is necessary to understand both the polarization and charge dynamics effects on their transconductance. Directly comparing ferroelectric Pb(Zr0.2Ti0.8)O3 and dielectric SrTiO3 field effect transistors, we show that the two effects strongly compete, with transient charge dynamics initially masking up to 40% of the ferroelectric field effect. For applications, it is therefore crucial to maximize the quality of the ferroelectric film and the interface with the carbon nanotube to take full advantage of the switchable polarization.
Ferroelectric domain switching in c-axis-oriented epitaxial Pb(Zr0.2Ti0.8)O3 thin films was studied using different field geometries and compared to numerical simulations and theoretical predictions. With carbon nanotubes as electrodes, continuous nanodomains as small as 9 nm in radius in a 270 nm thick film could be switched, remaining stable for over 20 months. Defect pinning of domain walls appears to play a key role in stabilizing such domains, below the predicted thermodynamic size limit.
We use electrostatic force microscopy and scanned gate microscopy to probe the conducting properties of carbon nanotubes at room temperature. Multi-walled carbon nanotubes are shown to be diffusive conductors, while metallic single-walled carbon nanotubes are ballistic conductors over micron lengths. Semiconducting single-walled carbon nanotubes are shown to have a series of large barriers to conduction along their length. These measurements are also used to probe the contact resistance and locate breaks in carbon nanotube circuits.
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 …
At any metal-carbon nanotube interface there is charge transfer and the induced interfacial field determines the position of the carbon nanotube band structure relative to the metal Fermi-level. In the case of a single-wall carbon nanotube (SWNT) supported on a gold substrate, we show that the charge transfers induce a local electrostatic potential perturbation which gives rise to the observed Fermi-level shift in scanning tunneling spectroscopy (STS) measurements. We also discuss the relevance of this study to recent experiments on carbon nanotube transistors and argue that the Fermi-level al…
Based on the similarity between the chiral nanotube and the classical solenoid, we study chiral transport along the circumferential direction in a carbon nanotube. We calculate the chiral conductivity, representing a circumferential current induced by an electric field along the nanotube axis for various chiralities of carbon nanotubes. We find that the chiral conductivity in a chiral nanotube is in general non zero, and oscillates as a function of the Fermi energy. This oscillating behavior is attributed to the subband structure of the nanotubes and the warping of the Fermi surfaces.
Electronic properties of metal-finite semiconducting carbon nanotube interfaces are studied as a function of the nanotube length using a self-consistent tight-binding theory. We find that the shape of the potential barrier depends on the long-range tail of the charge transfer, leading to an injection barrier thickness comparable to half of the nanotube length until the nanotube reaches the bulk limit. The conductance of the nanotube junction shows a transition from tunneling to thermally-activated transport with increasing nanotube length.
We present a detailed study of the static enhancement effects of electric charges in micron-length single-walled carbon nanotubes, using theoretically an atomic charge-dipole model and experimentally electrostatic force microscopy. We demonstrate that nanotubes exhibit at their ends surprisingly weak charge enhancements which decrease with the nanotube length and increase with the nanotube radius. A quantitative agreement is obtained between theory and experiments.
Electroabsorption spectroscopy of well-identified index-defined semiconducting carbon nanotubes is reported. The measurement of high definition electroabsorption spectra allows direct indexation with unique nanotube chirality. Results show that at least for a limited range of diameters, electroabsorption is directly proportional to the exciton binding energy of nanotubes. Electroabsorption is a powerful technique which directly probes into carbon nanotube excitonic states, and may become a useful tool for in situ study of excitons in future nanotube-based photonic devices such as electroabsorp…
The possibility for double-wall carbon nanotube to operate as the bolt and nut pair is studied. The barriers for relative motions of walls along the helical "thread" line and for jumps on neighbour helical lines are calculated as functions of wall lengths for the set of double-wall carbon nanotubes. The dynamics of relative motion of carbon nanotube walls along the helical line under the action of external forces is considered. Perforated nanodrill, variable nanoresistor and other principally new nanotube based mechanical nanodevices using these motion are proposed. Possible operation modes of…
The random phase approximation (RPA) theory is used to derive the Luttinger parameter g for metallic carbon nanotubes. The results are consistent with the Tomonaga-Luttinger models. All metallic carbon nanotubes, regardless if they are armchair tubes, zigzag tubes, or chiral tubes, should have the same Luttinger parameter g. However, a (10,10) carbon peapod should have a smaller g value than a (10,10) carbon nanotube. Changing the Fermi level by applying a gate voltage has only a second order effect on the g value. RPA theory is a valid approach to calculate plasmon energy in carbon nanotube s…
Spin transport in carbon-based materials has stimulated much interest due to their ballistic conductance and a long phase coherence length. While much research has been conducted on individual carbon nanotubes, current growth and placement techniques are incompatible with large-scale fabrication. Here we report nonlocal spin injection and detection in single wall carbon nanotube networks. We observe spin transport over a distance of 1 um, and extract a spin diffusion length of 1.6 - 2.4 um with an injected spin polarization from CoFe into nanotube network of 18 - 41%. Our observations demonstr…
We demonstrate that in a densely packed aligned array of single walled carbon nanotubes, the breakdown of one nanotube leads to a highly correlated breakdown of neighboring nanotubes, thereby producing a nano-fissure. We show that the origin of the correlation is the electrostatic field of the broken nanotubes that produces locally inhomogeneous current and Joule heating distributions in the neighboring intact nanotubes triggering their breakdowns in the vicinity of the broken nanotubes. Our results suggest that the densely aligned array behaves like a correlated solid.
Prompted by recent reports on $\sqrt{3} \times \sqrt{3}$ graphene superlattices with intrinsic inter-valley interactions, we perform first-principles calculations to investigate the electronic properties of periodically nitrogen-doped graphene and carbon nanotube nanostructures. In these structures, nitrogen atoms substitute one-sixth of the carbon atoms in the pristine hexagonal lattices with exact periodicity to form perfect $\sqrt{3} \times \sqrt{3}$ superlattices of graphene and carbon nanotubes. Multiple nanostructures of $\sqrt{3} \times \sqrt{3}$ graphene ribbons and carbon nanotubes ar…
We used tip-enhanced Raman spectroscopy to study the diameter-dependent Raman modes in a contacted carbon nanotube rope. We show that with the near-field tip enhancement a large number of nanotubes within a rope can be identified, even if the nanotube modes can not be distinguished in the far-field signal. Several metallic and semiconducting nanotubes can be identified and assigned to nanotube families. Additionally, we provide a tentative chiral index assignment.
Using single-nanotube absorption microscopy, we measured the absorption cross section of (6,5) carbon nanotubes at their second-order optical transition. We obtained a value of 3.2 10-17 cm2/C atom with a precision of 15% and an accuracy below 20%. This constitutes the first metrological investigation of the absorption cross section of chirality-identified nanotubes. Correlative absorption-luminescence microscopies performed on long nanotubes reveal a direct manifestation of exciton diffusion in the nanotube.
The unique topology and exceptional properties of carbon nanoscrolls (CNSs) have inspired unconventional nano-device concepts, yet the fabrication of CNSs remains rather challenging. Using molecular dynamics simulations, we demonstrate the spontaneous formation of a CNS from graphene on a substrate, initiated by a carbon nanotube (CNT). The rolling of graphene into a CNS is modulated by the CNT size, the carbon-carbon interlayer adhesion, and the graphene-substrate interaction. A phase diagram emerging from the simulations can offer quantitative guideline toward a feasible and robust physical …
We compute electrostatic fields induced deformations of cantilevered finite-length metallic carbon nanotubes, using an energy minimization method based on a charge-dipole moment interaction potential combined with an empirical many-body potential. The influence of field strength, field direction and tube geometry on the electrostatic deflection is investigated for both single and double walled tubes. These results could apply to nanoelectromechanical devices based on cantilevered carbon nanotubes.
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.
Although carbon nanotubes consist of honeycomb carbon, they have never been fabricated from graphene directly. Here, it is shown by quantum molecular-dynamics simulations and classical continuum-elasticity modeling, that graphene nanoribbons can, indeed, be transformed into carbon nanotubes by means of twisting. The chiralities of the tubes thus fabricated can be not only predicted but also externally controlled. This twisting route is an opportunity for nanofabrication, and is easily generalizable to ribbons made of other planar nanomaterials.
Recent years witnessed a rapid growth of interest of scientific and engineering communities to thermal properties of materials. Carbon allotropes and derivatives occupy a unique place in terms of their ability to conduct heat. The room-temperature thermal conductivity of carbon materials span an extraordinary large range - of over five orders of magnitude - from the lowest in amorphous carbons to the highest in graphene and carbon nanotubes. I review thermal and thermoelectric properties of carbon materials focusing on recent results for graphene, carbon nanotubes and nanostructured carbon mat…
We study the binding of chlorine atoms to carbon nanotubes and graphene at a Stone-Wales defect and to the sidewalls of pristine nanotubes. We show using ab initio thermodynamics that if the environment is chlorine-rich enough, the unzipping of carbon nanotubes into graphene nanoribbons with chlorinated edges may be thermodynamically feasible. By controlling the Cl chemical potential through temperature and pressure, opening selectively tubes below a threshold diameter might be possible. Additionally, we find increased binding energies for chlorine atoms bound to Stone-Wales defects as compare…
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.
We report the realization and characterization of independently controllable tunnel barriers within a carbon nanotube. The nanotubes are mechanically bent or kinked using an atomic force microscope, and top gates are subsequently placed near each kink. Transport measurements indicate that the kinks form gate-controlled tunnel barriers, and that gates placed away from the kinks have little or no effect on conductance. The overall conductance of the nanotube can be controlled by tuning the transmissions of either the kinks or the metal-nanotube contacts.
Local effects of multiple electrostatic gates placed beneath carbon nanotubes grown by chemical vapor deposition (CVD) are reported. Single-walled carbon nanotubes were grown by CVD from Fe catalyst islands across thin Mo "finger gates" (150 x 10nm). Prior to tube growth, several finger gates were patterned lithogrpahically and subsequently coated with a patterned high-k dielectric using low-temperature atomic layer deposition. Transport measurements demonstrate that local finger gates have a distinct effect from a global backgate.
The localization length and density of states of carbon nanotubes are evaluated within the tight-binding approximation. By comparison with the corresponding results for the square lattice tubes, it is found that the hexagonal structure affects strongly the behaviors of the density of states and localization lengths of carbon nanotubes.
We have studied tunneling of electrons into multi-wall carbon nanotubes. Nanotube/electrode interfaces with low transparency as well as nanotube/nanotube junctions created with atomic force microscope manipulation have been used. The tunneling conductance goes to zero as the temperature and bias are reduced, and the functional form is consistent with a power law suppression of tunneling as a function of energy. The exponent depends upon sample geometry. The relationship between these results and theories for tunneling into ballistic and disordered metals is discussed.
Long linear carbon chains encapsulated inside carbon nanotubes are a very close realization of carbyne, the truly one-dimensional allotrope of carbon. Here we study individual pairs of double-walled carbon nanotubes and encapsulated linear carbon chains by tip-enhanced Raman scattering. We observe that the radial breathing mode of the inner nanotube correlates with the frequency of the carbon chain's Raman mode, revealing that the nanotube chirality determines the vibronic and electronic properties of the encapsulated carbon chain. We provide the missing link that connects the properties of th…
We present ab initio calculations on the band structure and density of states of single wall semiconducting carbon nanotubes with high degrees (up to 25%) of B, Si and N substitution. The doping process consists of two phases: different carbon nanotubes (CNTs) for a constant doping rate and different doping rates for the zigzag (8, 0) carbon nanotube. We analyze the doping dependence of nanotubes on the doping rate and the nanotube type. Using these results, we select the zigzag (8, 0) carbon nanotube for toxic gas sensor calculation and obtain the total and partial densities of states for CNT…
In carbon nanotubes, the most abundant defects, caused for example by irradiation or chemisorption treatments, are small perturbing clusters, i.e. bi-site defects, extending over both A and B sites. The relative positions of these perturbing clusters play a crucial role in determining the electronic properties of carbon nanotubes. Using bandstructure and electronic transport calculations, we find out that in the case of armchair metallic nanotubes a band gap opens up when the clusters fulfill a certain periodicity condition. This phenomenon might be used in future nanoelectronic devices in whi…
We investigate the thermal conductivity of four types of deformed carbon nanotubes by using the nonequilibrium molecular dynamics method. It is reported that various deformations have different influence on the thermal properties of carbon nanotubes. For the bending carbon nanotubes, the thermal conductivity is independent on the bending angle. However, the thermal conductivity increases lightly with XY-distortion and decreases rapidly with Z-distortion. The thermal conductivity does not change with the screw ratio before the breaking of carbon nanotubes but decreases sharply after the critica…
The entanglement of two atoms (ions) doped into a carbon nanotube has been investigated theoretically. Based on the photon Green function formalism for quantizing electromagnetic field in the presence of carbon nanotubes, small-diameter metallic nanotubes are shown to result in a high degree of the two-qubit atomic entanglement for long times due to the strong atom-field coupling.
We use numerical simulations to analyze recent experimental measurements of short-channel carbon nanotube field-effect transistors with palladium contacts. We show that the gate strongly modulates the contact properties, an effect that is distinct from that observed in Schottky barrier carbon nanotube transistors. This modulation of the contacts by the gate allows for the realization of superior subthreshold swings for short channels, and improved scaling behavior. These results further elucidate the behavior of carbon nanotube-metal contacts, and should be useful in the optimization of high-p…
The objective of the present paper is to investigate the mechanical properties of carbon nanotubes. We use classical molecular dynamics simulation in order to study the effect of external compression, bending and torsion to nanotubes. We find that in the low temperature limit, the nanotubes are resilient, sustaining extreme strain without signs of brittleness or plasticity. For high temperatures and under tension the nanotubes show brittle or plastic behavior.
We develop the Bardeen-Cooper-Schrieffer (BCS) formalism for the superconductivity of carbon nanotubes. It is found that the superconducting transition temperature Tc of single-wall carbon nanotubes decreases exponentially with the increase of the tube diameter because the density of states near the Fermi energy is inversely proportional to the tube diameter. For the multi-wall carbon nanotubes, the Cooper paring hopping between layers enhances the superconducting correlation and increases the superconducting transition temperature, which is consistent with the experimental observation.
We propose a nonequilibrium Green's function approach to calculate the ac conductance of various finite-length carbon nanotubes. The simulated ac conductance differs significantly from that of the infinite-length ones. At the low-frequency limit, the profiles of the quantized conductance are still observable in the finite-length carbon nanotubes, but many more peaks appear on the conductance curves. We also show that the conductance of finite-length carbon nanotubes will oscillate as a function of the ac frequency. The dependence of the oscillation on the lengths, helicities and defects of the…
Extensive molecular dynamics simulations of water permeation and ion selectivity of the single-walled carbon nanotubes with the radial deformation are presented . The simulated results indicate that there is a close relationship between the minor axis of deformed carbon nanotubes and the variety, density as well as the position of functional groups. The critical minor axis of different diameter carbon nanotubes exists, and the carbon nanotube whose minor axis is less than the critical minor axis owns the selectivity of chlorine and sodium ions. Meanwhile, compared with intrinsic carbon nanotub…
Photonic crystal nanocavities are used to enhance photoluminescence from single-walled carbon nanotubes. Micelle-encapsulated nanotubes are deposited on nanocavities within Si photonic crystal slabs and confocal microscopy is used to characterize the devices. Photoluminescence spectra and images reveal nanotube emission coupled to nanocavity modes. The cavity modes can be tuned throughout the emission wavelengths of carbon nanotubes, demonstrating the ability to enhance photoluminescence from a variety of chiralities.
Two paramount challenges in carbon nanotube research are achieving chirality-controlled synthesis and understanding chirality-dependent device physics. High-throughput and in-situ chirality and electronic structural characterization of individual carbon nanotubes is crucial for addressing these challenges. Optical imaging and spectroscopy has unparalleled throughput and specificity, but its realization for single nanotubes on substrates or in devices has long been an outstanding challenge. Here we demonstrate video-rate imaging and in-situ spectroscopy of individual carbon nanotubes on various…
We analyze optical absorption by atomically doped carbon nanotubes with a special focus on the frequency range close to the atomic transition frequency. We derive the optical absorbtion line-shape function and, having analyzed particular achiral nanotubes of different diameters, predict the effect of absorbtion line splitting due to strong atom-vacuum-field coupling in small-diameter nanotubes. We expect this effect to stimulate relevant experimental efforts and thus to open a path to new device applications of atomically doped carbon nanotubes in modern nanotechnologies.
We have theoretically investigated electromechanical properties of freely suspended carbon nanotubes when a current is injected into the tubes using a scanning tunneling microscope. We show that a shuttle-like electromechanical instability can occur if the bias voltage exceeds a dissipation-dependent threshold value. An instability results in large amplitude vibrations of the carbon nanotube bending mode, which modify the current-voltage characteristics of the system.
With the use of the semiclassical Boltzmann equation we have calculated a direct current (d.c) in undoped zigzag carbon nanotube (CN) by mixing two coherent electromagnetic waves with commensurate frequencies i.e and . This effect is attributed to the nonparabolicity of the electron energy band which is very strong in carbon nanotubes. We observed that the current is negative similar to that observed in superlattice. However if the phase shift lies between and there is an inversion and the current becomes positive. It is interesting to note that exhibit negative differential conductivity as ex…
We report the first observation of trions (charged excitons), three-particle bound states consisting of one electron and two holes, in hole-doped carbon nanotubes at room temperature. When p-type dopants are added to carbon nanotube solutions, the photoluminescence and absorption peaks of the trions appear far below the E11 bright exciton peak, regardless of the dopant species. The unexpectedly large energy separation between the bright excitons and the trions is attributed to the strong electron-hole exchange interaction in carbon nanotubes.
We present a two-step procedure to probe hotspots of plasmon-enhanced Raman scattering with carbon nanotubes. Dielectrophoretic deposition places a small carbon nanotube bundle on top of plasmonic Au nanodimer. After 'pre-characterising' both the nanotubes and dimer structure, we subsequently use the tip of an AFM to push the bundle into the plasmonic hotspot located in the 25nm wide dimer gap, characterize its location inside the gap, and observe the onset of plasmon-enhanced Raman scattering. Evidence for the activation of the carbon nanotube's double-resonant D-mode by the near-field of the…
Deformations of single-wall carbon nanotubes are investigated within the tight-binding model with deformation-dependent hopping energies. We show that the nanotubes tend to twist and shrink spontaneously at zero temperature. The explicit values of the deformation parameters are computed for a wide range of nanotubes with varying diameter and chirality. The changes of the spectral gap associated with the spontaneous deformation are shown to depend on the chirality of the nanotubes.
A mechanism of stimulated emission of electromagnetic radiation by an electron beam in carbon nanotubes is theoretically considered. Three basic properties of carbon nanotubes, a strong slowing down of surface electromagnetic waves, ballisticity of the electron motion over typical nanotube length, and extremely high electron current density reachable in nanotubes, allow proposing them as candidates for the development of nano-scale Chernekov-type emitters, analogous to traveling wave tube and free electron laser. Dispersion equations of the electron beam instability and the threshold condition…
We present a comprehensive characterization of an individual multiwalled carbon nanotube transport device combining electron microscopy and Raman spectroscopy with electrical measurements. Each method gives complementary information that mutually help to interpret each other. A sample design that allows for combining these investigation methods on individual carbon nanotube devices is introduced. This offers a direct correlation of transport features and shifts of Raman modes with structural properties as e.g. the contact interface and the morphology of the nanotube.
The Rashba spin-orbit coupling in carbon nanotubes and its effect on spin-dependent transport properties are analyzed theoretically. We focus on clean non-interacting nanotubes with tunable number of subbands $N$. The peculiar band structure is shown to allow in principle for Datta-Das oscillatory behavior in the tunneling magnetoresistance as a function of gate voltage, despite the presence of multiple bands. We discuss the conditions for observing Datta-Das oscillations in carbon nanotubes.
The ability to tune the thermal resistance of carbon nanotube mechanical supports from insulating to conducting could permit the next generation of thermal management devices. Here, we demonstrate fabrication techniques for carbon nanotube supports that realize either weak or strong thermal coupling, selectively. Direct imaging by in-situ electron thermal microscopy shows that the thermal contact resistance of a nanotube weakly-coupled to its support is greater than 250 K*m/W and that this value can be reduced to 4.2(+5.6/-2.1) K*m/W by imbedding the nanotube in metal contacts.
We present an investigation of different thin-film evaporated ferromagnetic materials for their suitability as electrodes in individual single-wall and multi-wall carbon nanotube-based spin devices. Various electrode shapes made from permalloy (Ni_{81}Fe_{19}), the diluted ferromagnet PdFe, and PdFe/Fe bilayers are studied for both their micromagnetic properties and their contact formation to carbon nanotubes. Suitable devices are tested in low-temperature electron transport measurements, displaying the typical tunneling magnetoresistance of carbon nanotube pseudo spin valves.
Hysteretic switching in the magnetoresistance of short-channel, ferromagnetically contacted individual single wall carbon nanotubes is observed, providing strong evidence for nanotube spin transport. By varying the voltage on a capacitively coupled gate, the magnetoresistance can be reproducibly modified between +10% and -15%. The results are explained in terms of wave vector matching of the spin polarized electron states at the ferromagnetic / nanotube interfaces.
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 present atomically-resolved STM images of single-wall carbon nanotubes (SWNTs) embedded in a crystalline nanotube rope. Although they may be interpreted as of a chiral nanotube, the images are more consistently explained a an achiral armchair tube with a quenched twist distortion. The existence of quenched twists in SWNTs in ropes might explain the fact that both as-grown bulk nanotube material and individual ropes have insulator-like conductivity at low temperature.
Raman measurements in carbon allotropes are generally associated with the exploration of the vibrational modes. Here, we present a theory of the non-resonant inelastic light scattering accompanied by the excitations of intersubband electron-hole pairs in carbon nanotubes and predict the selection rules and polarization properties of the dominant intersubband Raman active modes.
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.
Photoluminescent carbon nanotubes are expected to become versatile room-temperature single-photon sources that have applications in quantum information processing. Quantum emission from carbon nanotubes is often induced by localization of excitons or exciton-exciton annihilation. Here, we modify the local energy landscape of excitons by decorating nanoscale pentacene particles onto air-suspended single-walled carbon nanotubes. Directional exciton diffusion from the undecorated region to the decorated site is demonstrated, suggesting exciton trapping induced by local dielectric screening from p…
