Tight binding description of the electronic response of a molecular device to an applied voltage

We analyze the effect of an external electric field on the electronic structure of molecules which have been recently studied as molecular wires or diodes. We use a self-consistent tight binding technique which provides results in good agreement with ab initio calculations and which may be applied to a large number of molecules. The voltage dependence of the molecular levels is mainly linear with slopes intimately related to the electronic structure of the molecules. We emphasize that the response to the applied voltage is an important feature which governs the behavior of a molecular device

Assessment of the notions of band offsets, wells and barriers at nanoscale semiconductor heterojunctions

Epitaxially-grown semiconductor heterostructures give the possibility to tailor the potential landscape for the carriers in a very controlled way. In planar lattice-matched heterostructures, the potential has indeed a very simple and easily predictable behavior: it is constant everywhere except at the interfaces where there is a step (discontinuity) which only depends on the composition of the semiconductors in contact. In this paper, we show that this universally accepted picture can be invalid in nanoscale heterostructures (e.g., quantum dots, rods, nanowires) which can be presently fabricated in a large variety of forms. Self-consistent tight-binding calculations applied to systems containing up to 75 000 atoms indeed demonstrate that the potential may have a more complex behavior in axial hetero-nanostructures: The band edges can show significant variations far from the interfaces if the nanostructures are not capped with a homogeneous shell. These results suggest new strategies to engineer the electronic properties of nanoscale objects, e.g. for sensors and photovoltaics.Comment: Accepted for publication in Phys. Rev.

Adsorption behavior of conjugated {C}3-oligomers on Si(100) and HOPG surfaces

A pi-conjugated {C}3h-oligomer involving three dithienylethylene branches bridged at the meta positions of a central benzenic core has been synthesized and deposited either on the Si(100) surface or on the HOPG surface. On the silicon surface, scanning tunneling microscopy allows the observation of isolated molecules. Conversely, by substituting the thiophene rings of the oligomers with alkyl chains, a spontaneous ordered film is observed on the HOPG surface. As the interaction of the oligomers is different with both surfaces, the utility of the Si(100) surface to characterize individual oligomers prior to their use into a 2D layer is discussed

Kekule versus hidden superconducting order in graphene-like systems: Competition and coexistence

We theoretically study the competition between two possible exotic superconducting orders that may occur in graphene-like systems, assuming dominant nearest-neighbor attraction: the gapless hidden superconducting order, which renormalizes the Fermi velocity, and the Kekule order, which opens a superconducting gap. We perform an analysis within the mean-field theory for Dirac electrons, at finite-temperature and finite chemical potential, as well as at half filling and zero-temperature, first excluding the possibility of the coexistence of the two orders. In that case, we find the dependence of the critical (more precisely, crossover) temperature and the critical interaction on the chemical potential. As a result of this analysis, we find that the Kekule order is preferred over the hidden order at both finite temperature and finite chemical potential. However, when the coexistence of the two superconducting orders is allowed, using the coupled mean-field gap equations, we find that above a critical value of the attractive interaction a mixed phase sets in, in which these orders coexist. We show that the critical value of the interaction for this transition is greater than the critical coupling for the hidden superconducting state in the absence of the Kekule order, implying that there is a region in the phase diagram where the Kekule order is favored as a result of the competition with the hidden superconducting order. The latter, however, eventually sets in and coexists with the Kekule state. According to our mean-field calculations, the transition from the Kekule to the mixed phase is of the second order, but it may become first order when fluctuations are considered. Finally, we investigate whether these phases could be possible in honeycomb superlattices of self-assembled semiconducting nanocrystals, which have been recently experimentally realized with CdSe and PbSe.Comment: 15 pages, 9 figures, published version. Minor changes, new references adde

Molecular rectifying diodes from self-assembly on silicon

We demonstrate a molecular rectifying junction made from a sequential self-assembly on silicon. The device structure consists of only one conjugated (p) group and an alkyl spacer chain. We obtain rectification ratios up to 37 and threshold voltages for rectification between -0.3V and -0.9V. We show that rectification occurs from resonance through the highest occupied molecular orbital of the p-group in good agreement with our calculations and internal photoemission spectroscopy. This approach allows us to fabricate molecular rectifying diodes compatible with silicon nanotechnologies for future hybrid circuitries

Modelling of spin decoherence in a Si hole qubit perturbed by a single charge fluctuator

Spin qubits in semiconductor quantum dots are one of the promizing devices to realize a quantum processor. A better knowledge of the noise sources affecting the coherence of such a qubit is therefore of prime importance. In this work, we study the effect of telegraphic noise induced by the fluctuation of a single electric charge. We simulate as realistically as possible a hole spin qubit in a quantum dot defined electrostatically by a set of gates along a silicon nanowire channel. Calculations combining Poisson and time-dependent Schr\"odinger equations allow to simulate the relaxation and the dephasing of the hole spin as a function of time for a classical random telegraph signal. We show that dephasing time $T_2$ is well given by a two-level model in a wide range of frequency. Remarkably, in the most realistic configuration of a low frequency fluctuator, the system has a non-Gaussian behavior in which the phase coherence is lost as soon as the fluctuator has changed state. The Gaussian description becomes valid only beyond a threshold frequency $\omega_{th}$, when the two-level system reacts to the statistical distribution of the fluctuator states. We show that the dephasing time $T_{2}(\omega_{th})$ at this threshold frequency can be considerably increased by playing on the orientation of the magnetic field and the gate potentials, by running the qubit along "sweet" lines. However, $T_{2}(\omega_{th})$ remains bounded due to dephasing induced by the non-diagonal terms of the stochastic perturbation Hamiltonian. Our simulations reveal that the spin relaxation cannot be described cleanly in the two-level model because the coupling to higher energy hole levels impacts very strongly the spin decoherence. This result suggests that multi-level simulations including the coupling to phonons should be necessary to describe the relaxation phenomenon in this type of qubit

Quantum confinement effects in Pb Nanocrystals grown on InAs

In the recent work of Ref.\cite{Vlaic2017-bs}, it has been shown that Pb nanocrystals grown on the electron accumulation layer at the (110) surface of InAs are in the regime of Coulomb blockade. This enabled the first scanning tunneling spectroscopy study of the superconducting parity effect across the Anderson limit. The nature of the tunnel barrier between the nanocrystals and the substrate has been attributed to a quantum constriction of the electronic wave-function at the interface due to the large Fermi wavelength of the electron accumulation layer in InAs. In this manuscript, we detail and review the arguments leading to this conclusion. Furthermore, we show that, thanks to this highly clean tunnel barrier, this system is remarkably suited for the study of discrete electronic levels induced by quantum confinement effects in the Pb nanocrystals. We identified three distinct regimes of quantum confinement. For the largest nanocrystals, quantum confinement effects appear through the formation of quantum well states regularly organized in energy and in space. For the smallest nanocrystals, only atomic-like electronic levels separated by a large energy scale are observed. Finally, in the intermediate size regime, discrete electronic levels associated to electronic wave-functions with a random spatial structure are observed, as expected from Random Matrix Theory.Comment: Main 12 pages, Supp: 6 page

Phonon-limited carrier mobility and resistivity from carbon nanotubes to graphene

Under which conditions do the electrical transport properties of one-dimensional (1D) carbon nanotubes (CNTs) and 2D graphene become equivalent? We have performed atomistic calculations of the phonon-limited electrical mobility in graphene and in a wide range of CNTs of different types to address this issue. The theoretical study is based on a tight-binding method and a force-constant model from which all possible electron-phonon couplings are computed. The electrical resistivity of graphene is found in very good agreement with experiments performed at high carrier density. A common methodology is applied to study the transition from 1D to 2D by considering CNTs with diameter up to 16 nm. It is found that the mobility in CNTs of increasing diameter converges to the same value, the mobility in graphene. This convergence is much faster at high temperature and high carrier density. For small-diameter CNTs, the mobility strongly depends on chirality, diameter, and existence of a bandgap.Comment: 12 page