Quantum interference in atomic-sized point contacts

The conductance of atomic-sized metallic point contacts is shown to be strongly voltage dependent due to quantum interference with impurities even in samples with low impurity concentrations. Transmission through these small contacts depends not only on the local atomic structure at the contact but also on the distribution of impurities or defects within a coherence length of the contact. In contrast with other mesoscopic systems we show that transport through atomic contacts is coherent even at room temperature. The use of a scanning tunneling microscope (STM) makes it possible to fabricate one atom contacts of gold whose transmission can be controlled by manipulation of the contact allowing inelastic spectroscopy in such small contacts.

Quantum Dot-Sensitized Solar Cells Based on Directly Adsorbed Zinc Copper Indium Sulfide Colloids

Heavy metal-based quantum dots (QDs) have demonstrated to behave as efficient sensitizers in QD-sensitized solar cells (QDSSCs), as attested by the countless works and encouraging efficiencies reported so far. However, their intrinsic toxicity has arisen as a major issue for the prospects of commercialization. Here, we examine the potential of environmentally friendly zinc copper indium sulfide (ZCIS) QDs for the fabrication of liquid-junction QDSSCs by means of photoelectrochemical measurements. A straightforward approach to directly adsorb ZCIS QDs on TiO2 from a colloidal dispersion is presented. Incident photon-to-current efficiency (IPCE) spectra of sensitized photoanodes show a marked dependence on the adsorption time, with longer times leading to poorer performances. Cyclic voltammograms point to a blockage of the channels of the mesoporous TiO2 film by the agglomeration of QDs as the main reason for the decrease in efficiency. Photoanodes were also submitted to the ZnS treatment. Its effects on electron recombination with the electrolyte are analyzed through electrochemical impedance spectroscopy and photopotential measurements. The corresponding results bring out the role of the ZnS coating as a barrier layer preventing electron leakage toward the electrolyte, as argued in other QD-sensitized systems. The beneficial effect of the ZnS coating is ultimately reflected on the power conversion efficiency of complete devices, reaching values of 2 %. In a more general vein, through these findings, we aim to call the attention to the potentiality of this quaternary alloy, virtually unexplored as a light harvester for sensitized devices.

Quantum spin Hall phase in multilayer graphene

The so-called quantum spin Hall phase is a topologically nontrivial insulating phase that is predicted to appear in graphene and graphenelike systems. In this paper we address the question of whether this topological property persists in multilayered systems. We consider two situations: purely multilayer graphene and heterostructures where graphene is encapsulated by trivial insulators with a strong spin-orbit coupling. We use a four-orbital tight-binding model that includes full atomic spin-orbit coupling and we calculate the Z2 topological invariant of the bulk states as well as the edge states of semi-infinite crystals with armchair termination. For homogeneous multilayers we find that even when the spin-orbit interaction opens a gap for all possible stackings, only those with an odd number of layers host gapless edge states while those with an even number of layers are trivial insulators. For heterostructures where graphene is encapsulated by trivial insulators, it turns out that interlayer coupling is able to induce a topological gap whose size is controlled by the spin-orbit coupling of the encapsulating materials, indicating that the quantum spin Hall phase can be induced by proximity to trivial insulators.

Can model Hamiltonians describe the electron–electron interaction in π-conjugated systems?: PAH and graphene

Model Hamiltonians have been, and still are, a valuable tool for investigating the electronic structure of systems for which mean field theories work poorly. This review will concentrate on the application of Pariser–Parr–Pople (PPP) and Hubbard Hamiltonians to investigate some relevant properties of polycyclic aromatic hydrocarbons (PAH) and graphene. When presenting these two Hamiltonians we will resort to second quantisation which, although not the way chosen in its original proposal of the former, is much clearer. We will not attempt to be comprehensive, but rather our objective will be to try to provide the reader with information on what kinds of problems they will encounter and what tools they will need to solve them. One of the key issues concerning model Hamiltonians that will be treated in detail is the choice of model parameters. Although model Hamiltonians reduce the complexity of the original Hamiltonian, they cannot be solved in most cases exactly. So, we shall first consider the Hartree–Fock approximation, still the only tool for handling large systems, besides density functional theory (DFT) approaches. We proceed by discussing to what extent one may exactly solve model Hamiltonians and the Lanczos approach. We shall describe the configuration interaction (CI) method, a common technology in quantum chemistry but one rarely used to solve model Hamiltonians. In particular, we propose a variant of the Lanczos method, inspired by CI, that has the novelty of using as the seed of the Lanczos process a mean field (Hartree–Fock) determinant (the method will be named LCI). Two questions of interest related to model Hamiltonians will be discussed: (i) when including long-range interactions, how crucial is including in the Hamiltonian the electronic charge that compensates ion charges? (ii) Is it possible to reduce a Hamiltonian incorporating Coulomb interactions (PPP) to an 'effective' Hamiltonian including only on-site interactions (Hubbard)? The performance of CI will be checked on small molecules. The electronic structure of azulene and fused azulene will be used to illustrate several aspects of the method. As regards graphene, several questions will be considered: (i) paramagnetic versus antiferromagnetic solutions, (ii) forbidden gap versus dot size, (iii) graphene nano-ribbons, and (iv) optical properties.

Edge states in graphene-like systems

The edges of graphene and graphene like systems can host localized states with evanescent wave function with properties radically different from those of the Dirac electrons in bulk. This happens in a variety of situations, that are reviewed here. First, zigzag edges host a set of localized non-dispersive state at the Dirac energy. At half filling, it is expected that these states are prone to ferromagnetic instability, causing a very interesting type of edge ferromagnetism. Second, graphene under the influence of external perturbations can host a variety of topological insulating phases, including the conventional quantum Hall effect, the quantum anomalous Hall (QAH) and the quantum spin Hall phase, in all of which phases conduction can only take place through topologically protected edge states. Here we provide an unified vision of the properties of all these edge states, examined under the light of the same one orbital tight-binding model. We consider the combined action of interactions, spin–orbit coupling and magnetic field, which produces a wealth of different physical phenomena. We briefly address what has been actually observed experimentally.