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We present a non-reactive force field for molecular dynamics simulations of interfaces between passivated amorphous surfaces and their interaction with water. The force field enables large-scale dynamic simulations of dry and lubricated tribological contacts and is tailored to surfaces with hydrogen, hydroxyl and aromatic surface passivation. To favour its compatibility with existing force-field parameterizations for liquids and allow a straightforward extension to other types of surface passivation species, we adopt the commonly used OPLS functional form. The optimisation of the force-field parameters is systematic and follows a protocol that can be reused for other surface-molecule combinations. Reference data are calculated with gradient- and dispersion-corrected density functional theory and include the bonding structure and elastic deformation of bulk and surface structures as well as surface adhesion and water adsorption energy landscapes. The conventions adopted to define the different force-field atom types are based on the hybridisation of carbon orbitals and enable a simple and efficient parameter optimisation strategy based on quantum-mechanical calculations performed only on crystalline reference structures. Transferability tests on amorphous interfaces demonstrate the effectiveness of this approach. After testing the force field, we present two examples of application to tribological problems. Namely, we investigate relationships between dry friction and the corrugation of the contact potential energy surface and the dependency of friction on the thickness of interface water films. We finally discuss the limitations of the force field and propose strategies for its improvement and extension.

We show that quantum confinement in the valence and conduction bands of semiconducting single-walled carbon nanotubes can be engineered by means of artificial defects. This ability holds potential for designing future nanotube-based quantum devices such as electrically driven room-temperature single-photon sources emitting at telecom-wavelength. Using Ar$^{+}$ and N$^{+}$ ion-induced defects, intrananotube quantum dots with sub-10 nm lateral sizes are created, giving rise to quantized electronic bound states with level spacings of the order of 100 meV and larger. Using low-temperature scanning tunneling spectroscopy, we resolve the energy and real space properties of the quantized states and compare them with theoretical model calculations. By solving the Schr\"odinger equation over a one-dimensional piecewise constant potential model, the effects of inhomogeneous defect scattering strength as well as surface variations in the Au(111) substrate on the quantized states structure are remarkably well reproduced. Furthermore, using ab-initio calculations, we demonstrate that defect structures such as vacancies, di-vacancies and chemisorbed nitrogen ad-atoms constitute strong scattering centers able to form quantum dots with clear signatures of discrete bound states as observed experimentally. The ab-initio simulations also allowed to study the scattering strength profile as a function of energy for different defect combinations, supporting the potential of highly stable double vacancies for practical applications at room temperature., Comment: Supplementary Informations can be downloaded at the following link: http://dario-bercioux.eu/download/SM/Supp_info.pdf

The breaking of symmetry is the ground on which many physical phenomena are explained. This is important in particular for bipartite lattice structure as graphene and carbon nanotubes, where particle-hole and pseudo-spin are relevant symmetries. Here we investigate the role played by the defect-induced breaking of these symmetries in the electronic scattering properties of armchair single-walled carbon nanotubes. From Fourier transform of the local density of states we show that the active electron scattering channels depend on the conservation of the pseudo-spin. Further, we show that the lack of particle-hole symmetry is responsible for the pseudo-spin selection rules observed in several experiments. This symmetry breaking arises from the lattice reconstruction appearing at defect sites. Our analysis gives an intuitive way to understand the scattering properties of carbon nanotubes, and can be employed for newly interpret several experiments on this subject. Further, it can be used to design devices such as pseudo-spin filter by opportune defect engineering.

We investigate spin effects in transport across fully interacting, finite size graphene armchair nanoribbons (ACNs) contacted to collinearly spin-polarized leads. In such systems, the presence of short ranged Coulomb interaction between bulk states and states localized at the ribbon ends leads to novel spin-dependent phenomena. Specifically, the total spin of the low energy many-body states is conserved during tunneling but that of the bulk and end states is not. As a consequence, in the single-electron regime, dominated by Coulomb blockade phenomena, we find pronounced negative differential conductance features for ACNs contacted to parallel polarized leads. These features are however absent for an anti-parallel contact configuration, which in turn leads within a certain gate and bias voltage region to a negative tunneling magneto-resistance. Moreover, we analyze the changes in the transport characteristics under the influence of an external magnetic field., Comment: 37 pages, 9 figures, 2 tables; revised published version

We investigate linear and nonlinear transport across single-walled carbon nanotube quantum dots weakly coupled to spin-polarized leads. We consider tubes of finite length and small diameter, where not only forward scattering contributions of the Coulomb potential, but also short-ranged processes play an important role. In particular, they induce exchange effects leading for electron fillings 4n+2 either to a non-degenerate groundstate of spin S=0 or to a triplet groundstate. In the linear regime we present analytical results for the conductance - for both the S=0 and the triplet groundstate - and demonstrate that an external magnetic field is crucial to reveal the spin nature of the groundstates. In the nonlinear regime we show stability diagrams that clearly distinguish between the different groundstates. We observe a negative differential conductance (NDC) effect in the S=0 groundstate for antiparallel lead magnetization. In presence of an external magnetic field spin blockade effects can be detected, again leading to NDC effects for both groundstates., Comment: 13 pages, 15 figures, 2 tables; revised published version

We present a microscopic theory for interacting graphene armchair nanoribbon quantum dots. Long range interaction processes are responsible for Coulomb blockade and spin-charge separation. Short range ones, arising from the underlying honeycomb lattice of graphene, smear the spin-charge separation and induce exchange correlations between bulk electrons - delocalized on the ribbon - and single electrons localized at the two ends. As a consequence, entangled end-bulk states where the bulk spin is no longer a conserved quantity occur. Entanglement's signature is the occurrence of negative differential conductance effects in a fully symmetric set-up due to symmetry-forbidden transitions., Comment: 6 pages, 7 figures; version submitted to EPL

The low energy spectrum of finite size metallic single-walled carbon nanotubes SWNTs) is determined. Starting from a tight binding model for the $p_{z}$ electrons, we derive the low energy Hamiltonian containing all relevant scattering processes resulting from the Coulomb interaction, including the short ranged contributions becoming relevant for small diameter tubes. In combination with the substructure of the underlying honeycomb lattice the short ranged processes lead to various exchange effects. Using bosonization the spectrum is determined. We find that the ground state is formed by a spin 1 triplet, if $4n+2$ electrons occupy the SWNT and the branch mismatch is smaller than the exchange splitting. Additionally, we calculate the excitation spectra for the different charge states and find the lifting of spin-charge separation as well as the formation of a quasi-continuum at higher excitation energies., Comment: European Physical Journal B (2008) in press

The electronic spectrum of metallic finite-size single-wall carbon nanotubes at low energies is derived. It is based on a tight-binding description for the interacting p_{z} electrons. Not only the forward scattering parts of the Coulomb interaction, which are diagonalized by bosonization, are considered, but also all other processes becoming relevant for small diameter tubes. As a consequence of the substructure of the underlying lattice, a spin 1 triplet is found as ground state if the exchange splitting is larger than the branch mismatch, a spin 0 singlet otherwise. Moreover the excitation spectrum is calculated.

We investigate linear and nonlinear transport in interacting single wall carbon nanotubes (SWCNTs) that are weakly attached to ferromagnetic leads. For the reduced density matrix of a SWCNT quantum dot, equations of motion which account for an arbitrarily vectored polarisation of the contacts are derived. We focus on the case of large diameter nanotubes where exchange effects emerging from short-ranged processes can be excluded and the four-electron periodicity at low bias can be observed. This yields in principle four distinct resonant tunnelling regimes, but due to symmetries in the involved groundstates, each two possess a mirror-symmetry. With a non-collinear configuration, we recover at the 4N <-> 4N+1 / 4N+3 <-> 4N resonances the analytical results known for the angular dependence of the conductance of a single level quantum dot or a metallic island. The two other cases are treated numerically and show on the first glance similar, yet not analytically describable dependences. In the nonlinear regime, negative differential conductance features occur for non-collinear lead magnetisations., Comment: 39 pages, 19 figures; revised final published version

We present a low energy-theory for non-linear transport in finite-size interacting single-wall carbon nanotubes. It is based on a microscopic model for the interacting p_z electrons and successive bosonization. We consider weak coupling to the leads and derive equations of motion for the reduced density matrix. We focus on the case of large-diameter nanotubes where exchange effects can be neglected. In this situation the energy spectrum is highly degenerate. Due to the multiple degeneracy, diagonal as well as off-diagonal (coherences) elements of the density matrix contribute to the nonlinear transport. At low bias, a four-electron periodicity with a characteristic ratio between adjacent peaks is predicted. Our results are in quantitative agreement with recent experiments.

A low energy-theory for non-linear transport in finite-size single-wall carbon nanotubes, based on a microscopic model for the interacting pz electrons and successive bosonization, is presented. Due to the multiple degeneracy of the energy spectrum diagonal as well as off-diagonal (coherences) elements of the reduced density matrix contribute to the nonlinear transport. A four-electron periodicity with a characteristic ratio between adjacent peaks, as well as nonlinear transport features, in quantitative agreement with recent experiments, are predicted., Comment: 5 pages, 3 figures