Exciton binding energies in carbon nanotubes from two-photon photoluminescence

One- and two-photon luminescence excitation spectroscopy showed a series of distinct excitonic states in single-walled carbon nanotubes. The energy splitting between one- and two-photon-active exciton states of different wavefunction symmetry is the fingerprint of excitonic interactions in carbon nanotubes. We determine exciton binding energies of 0.3-0.4 eV for different nanotubes with diameters between 0.7 and 0.9 nm. Our results, which are supported by ab-initio calculations of the linear and non-linear optical spectra, prove that the elementary optical excitations of carbon nanotubes are strongly Coulomb-correlated, quasi-one dimensionally confined electron-hole pairs, stable even at room temperature. This alters our microscopic understanding of both the electronic structure and the Coulomb interactions in carbon nanotubes, and has direct impact on the optical and transport properties of novel nanotube devices.Comment: 5 pages, 4 figure

Extraordinary sensitivity of the electronic structure and properties of single-walled carbon nanotubes to molecular charge-transfer

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.Comment: 15 pages, 5 figurre

Chemical reactivity imprint lithography on graphene: Controlling the substrate influence on electron transfer reactions

The chemical functionalization of graphene enables control over electronic properties and sensor recognition sites. However, its study is confounded by an unusually strong influence of the underlying substrate. In this paper, we show a stark difference in the rate of electron transfer chemistry with aryl diazonium salts on monolayer graphene supported on a broad range of substrates. Reactions proceed rapidly when graphene is on SiO_2 and Al_2O_3 (sapphire), but negligibly on alkyl-terminated and hexagonal boron nitride (hBN) surfaces. The effect is contrary to expectations based on doping levels and can instead be described using a reactivity model accounting for substrate-induced electron-hole puddles in graphene. Raman spectroscopic mapping is used to characterize the effect of the substrates on graphene. Reactivity imprint lithography (RIL) is demonstrated as a technique for spatially patterning chemical groups on graphene by patterning the underlying substrate, and is applied to the covalent tethering of proteins on graphene.Comment: 25 pages, 6 figure

Relaxation dynamics of carbon nanotubes of enriched chiralities

In our work we combined experimental and theoretical investigations of the relaxation dynamics of the single wall carbon nanotubes (SW-CNTs) in solution samples with enriched chiralities of (7,5) and (7,6) species. In two-color pump-probe studies we observe three-exponential decay in the differential transmission spectra in the range of few picoseconds, tens of picoseconds, and hundreds of picoseconds. Decay curves are very similar for both SW-CNT chiralities under resonant excitation and probing of excited and ground state transition energies, respectively. Both types of tubes exhibit no changes in decay for the different excitation energies in the range ±50meV around the excited state. By tuning the probe pulse towards energies higher then ground state (up to +350meV) we observe acceleration of the first decay component from 5.8ps down to 1.6ps. Our experimental results are supported by time resolved microscopic calculations based on carbon nanotube Bloch equations proving the fast decay component behavior being dominated through scattering with acoustic phonons

Mechanisms of titania nanoparticle mediated growth of turbostratic carbon nanotubes and nanofibers

Turbostratic carbon nanotubes (CNTs) and nanofibers (CNFs) are synthesized by chemical vapor deposition using titania nanoparticle catalysts, and a quantitative lift-off model is developed to explain CNT and CNF growth. Micron-scale long turbostratic CNTs and CNFs were observed when acetylene is utilized as a carbon feedstock, and an alumina substrate was incorporated to improve the homogeneity of catalyst distribution. Turbostratic CNTs/CNFs are always found attached to nanoparticle corners, in the absence of the graphitic cage that is typically observed with metal nanoparticle-mediated growth. The observed morphology in turbostratic CNTs/CNFs supports a model in which several layers of graphene lift off from high-curvature corners of the titania nanoparticle catalysts. This model explains a key feature, which differentiates the growth of turbostratic CNTs/CNFs via non-metallic nanoparticles from growth using standard metal nanoparticle catalysts. The observed CNT/CNF growth and the accompanying model can impact the assessment of other metal-oxide nanoparticle catalysts, with the findings here contributing to a metal-free synthesis of turbostratic CNTs/CNFs

Molecular Valves for Controlling Gas Phase Transport Made from Discrete Angstrom-Sized Pores in Graphene

An ability to precisely regulate the quantity and location of molecular flux is of value in applications such as nanoscale 3D printing, catalysis, and sensor design. Barrier materials containing pores with molecular dimensions have previously been used to manipulate molecular compositions in the gas phase, but have so far been unable to offer controlled gas transport through individual pores. Here, we show that gas flux through discrete angstrom-sized pores in monolayer graphene can be detected and then controlled using nanometer-sized gold clusters, which are formed on the surface of the graphene and can migrate and partially block a pore. In samples without gold clusters, we observe stochastic switching of the magnitude of the gas permeance, which we attribute to molecular rearrangements of the pore. Our molecular valves could be used, for example, to develop unique approaches to molecular synthesis that are based on the controllable switching of a molecular gas flux, reminiscent of ion channels in biological cell membranes and solid state nanopores.Comment: to appear in Nature Nanotechnolog

Raman excitation profile of the G band in single-chirality carbon nanotubes

We present in this work measurements of the Raman excitation profile of the high-energy phonons (G band) in single-chirality (n,m) semiconducting single-wall carbon nanotubes using more than 70 laser excitation energies, and a theoretical description based on the third-order quantum model for Raman scattering. We show that the observed asymmetry in the G band Raman excitation profile is rigorously explained by considering all physical elements associated with Raman scattering in (n,m) carbon nanotubes, such as the existence of van Hove singularities in the electronic density of states and wave-vector dependence of the matrix elements of the Raman process. We conclude that the proposed violation of the Condon approximation is not a fundamental principle underlying the nanotube photophysics

A comparative analysis of Australian and Hong Kong retirement systems

In the developed world, there comes a point in a person’s life when it is socially accepted that they should no longer be required to earn an income through personal exertion — generally quantitatively determined by their age. The level of support an older person receives is often correlated with the economic stability of the jurisdiction in which they reside. This support can range from basic services through to modest level pensions and healthcare. All support is funded by government revenue (i.e. taxes). Such revenue is predominately derived through taxpayers and, most notably, the working population. A large issue affecting countries globally is that of aging populations. Statistically, older persons are considered to be those over the age of 60. Aging populations are a direct result of increased mortality rates followed by reductions in fertility rates. The financial impact of aging populations is that a large network of people finds themselves being supported by a much smaller network. This places a greater burden on the younger population and risks a lower standard of living for older people.To combat the economic and social risks associated with an aging population, many countries over the past decade have implemented significant pension reforms which have included increasing age requirements for pension benefits, changing the way in which entitlements are calculated and introducing compulsory savings. The World Bank’s leading involvement in pension reform, globally, has identified that the main objectives of a pension system continues to be poverty alleviation and consumption smoothing — beneath the umbrella of social protection. This paper reviews each comparator country’s retirement income system using the World Banks Pension Conceptual Framework. It then considers each country’s system in terms such as adequacy, affordability, sustainability, equitability, predictability and robustness

Evidence of dynamical dipole excitation in the fusion-evaporation of the 40Ca +152Sm heavy system

The excitation of the dynamical dipole mode along the fusion path was investigated for the first time in the formation of a heavy compound nucleus in the A ∼ 190 mass region. The compound nucleus was formed at identical conditions of excitation energy and spin from two entrance channels: the charge-asymmetric 40 Ca + 152 Sm and the nearly charge-symmetric 48 Ca + 144 Sm at E lab = 11 and 10.1 MeV / nucleon, respectively. High-energy γ rays and light charged particles were measured in coincidence with evaporation residues by means of the MEDEA multidetector array (Laboratori Nazionali del Sud, Italy) coupled to four parallel plate avalanche counters. The charged particle multiplicity spectra and angular distributions were used to pin down the average excitation energy, the average mass, and the average charge of the compound nucleus. The γ -ray multiplicity spectrum and angular distribution related to the nearly charge-symmetric channel were employed to obtain new data on the giant dipole resonance in the compound nucleus. The dynamical dipole mode excitation in the charge-asymmetric channel was evidenced, in a model-independent way, by comparing the γ -ray multiplicity spectra and angular distributions of the two entrance channels with each other. Calculations of the dynamical dipole mode in the 40 Ca + 152 Sm channel, based on a collective bremsstrahlung analysis of the reaction dynamics, are presented. Possible interesting implications in the superheavy-element quest are discussed

Halo effects on fusion cross section in 4,6He+64Zn collision around and below the Coulomb barrier

The structure of the halo nuclei is expected to influence the fusion mechanism at energies around and below the Coulomb barrier. Here new data of 4He+64Zn at sub-barrier energies are presented which cover the same energy region of previous measurements of 6He+64Zn. The fusion cross section was measured by using an activation technique where the radioactive evaporation residues produced in the reaction were identified by the X-ray emission which follows their electron capture decay. By comparing the two system, we observe an enhancement on the fusion cross section in the reaction induced by 6He, at energy below the Coulomb barrier. It is shown that this enhancement seems to be due to static properties of halo 2n 6He nucleus