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In this paper, the atomic layer deposition (ALD) of ultra-thin films (<4 nm) of $Al_{2}O_{3}$ and $HfO_{2}$ on Au-supported monolayer (1L) $MoS_{2}$ is investigated, providing an insight on the nucleation mechanisms in the early stages of the ALD process. A preliminary multiscale characterization of large area 1L-$MoS_{2}$ exfoliated on sputter-grown Au/Ni films revealed an almost conformal $MoS_{2}$ membrane with the Au topography and the occurrence of strain variations at the nanoscale. Ab-initio DFT calculations of $MoS_{2}$/Au(111) interface showed a significant influence of the Au substrate on the $MoS_{2}$ energy band structure, whereas small differences were accounted for the adsorption of the $H_{2}O$, TMA and TDMAHf precursors. This suggests a crucial role of nanoscale morphological effects, such as local curvature and strain of the $MoS_{2}$ membrane, in the enhanced physisorption of the precursors. Therefore, the nucleation and growth of $Al_{2}O_{3}$ and $HfO_{2}$ films onto 1L-$MoS_{2}$/Au was investigated, by monitoring the surface coverage as a function of the number (N) of ALD cycles, with N from 10 to 120. At low N values, a slower growth rate of the initially formed nuclei was observed for $HfO_{2}$, probably due to the bulky nature of the TDMAHf precursor as compared to TMA. On the other hand, the formation of continuous films was obtained in both cases for N>80 ALD cycles, corresponding to 3.6 nm $Al_{2}O_{3}$ and 3.1 nm $HfO_{2}$. Current mapping by C-AFM showed, for the same applied bias, a uniform insulating behavior of $Al_{2}O_{3}$ and the occurrence of few localized breakdown spots in the case of $HfO_{2}$, associated to less compact films regions. Finally, an increase of the 1L-$MoS_{2}$ tensile strain was observed by Raman mapping after encapsulation with both high-k films, accompanied by a reduction in the PL intensity., Comment: 26 pages, 9 figures

We present a stochastic simulation method designed to study at an atomic resolution the growth kinetics of compounds characterized by the sp3-type bonding symmetry. Formalization and implementation details are discussed for the particular case of the 3C-SiC material. A key feature of our numerical tool is the ability to simulate the evolution of both point-like and extended defects, whereas atom kinetics depend critically on process-related parameters. In particular, the simulations can describe the surface state of the crystal and the generation/evolution of defects as a function of the initial substrate condition and the calibration of the simulation parameters. We demonstrate that quantitative predictions of the microstructural evolution of the studied systems can be readily compared with the structural characterization of actual processed samples.

In spite of its great promises for energy efficient power conversion, the electronic quality of cubic silicon carbide (3C-SiC) on silicon is currently limited by the presence of a variety of extended defects in the heteroepitaxial material. However, the specific role of the different defects on the electronic transport is still under debate. In this work, a macro- and nano-scale characterization of Schottky contacts on 3C-SiC/Si was carried out, to elucidate the impact of the anti-phase-boundaries (APBs) and stacking-faults (SFs) on the forward and reverse current-voltage characteristics of these devices. Current mapping of 3C-SiC by conductive atomic force microscopy (CAFM) directly showed the role of APBs as the main defects responsible of the reverse bias leakage, while both APBs and SFs were shown to work as preferential current paths under forward polarization. Distinct differences between these two kinds of defects were also confirmed by electronic transport simulations of a front-to-back contacted SF and APB. These experimental and simulation results provide a picture of the role played by different types of extended defects on the electrical transport in vertical or quasi-vertical devices based on 3C-SiC/Si, and can serve as a guide for improving material quality by defects engineering., Comment: 20 pages, 7 figures

We study coherent backscattering phenomena from single and multiple stacking faults (SFs) in 3C- and 4H-SiC within density functional theory quantum transport calculations. We show that SFs give rise to highly dispersive bands within both the valance and conduction bands that can be distinguished for their enhanced density of states at particular wave number subspaces. The consequent localized perturbation potential significantly scatters the propagating electron waves and strongly increases the resistance for $n$-doped systems. We argue that resonant scattering from SFs should be one of the principal degrading mechanisms for device operation in silicon carbide., Comment: 5 pages, 4 figures

We present an orbital-resolved density functional theory study on the electronic properties of hydrogen and lithium intercalated graphene grown on the Si face of SiC. Starting from the $(6\sqrt3\times6\sqrt3)R30^{\circ}$ surface reconstruction of the graphene/SiC heterosystem, we find that both H and Li can restore the ideal structural characteristics of the two nonequivalent junction parts (i.e. graphene and the SiC substrate) when inserted at the interface. However, the chemical/electrostatic interactions remain different for the two cases. Hence, H-intercalated epitaxial graphene is subject to a sublattice symmetry-breaking electronic interference that perturbs the Dirac point, whereas Li intercalation gives rise to a highly $n$-doped system due to a nonuniform delocalization of Li charges. Results bring to discussion the role of substrate engineering in epitaxial graphene on SiC., Comment: 6 pages, 4 figures, accepted in PRB

We perform density functional theory calculations for the determination of the structural and electronic properties of epitaxial graphene on 4H-SiC(000$\bar{1}$). Using commensurate supercells that minimize non-physical stresses we show that, in contrast with Si-face epitaxial films, the first graphene layer that forms on the C-face of SiC is purely metallic with its $\pi$-bands partially preserved. Typical free-standing characteristics are fully recovered with a second graphene layer. We moreover discuss on the magnetic properties of the interface and the absence of Fermi-level pinning effects that could allow for a plausible device operation starting from the off-state., Comment: 4 pages, 4 figures

We calculate quantum transport for metal-graphene nanoribbon heterojunctions within the atomistic self-consistent Schr\"odinger/Poisson scheme. Attention is paid on both the chemical aspects of the interface bonding as well the one-dimensional electrostatics along the ribbon length. Band-bending and doping effects strongly influence the transport properties, giving rise to conductance asymmetries and a selective suppression of the subband formation. Junction electrostatics and p-type characteristics drive the conduction mechanism in the case of high work function Au, Pd and Pt electrodes, while contact resistance becomes dominant in the case of Al., Comment: 4 pages, 5 figures

We present a systematic study of electron backscattering phenomena during conduction for graphene nanoribbons with single-vacancy scatterers and dimensions within the capabilities of modern lithographic techniques. Our analysis builds upon an \textit{ab initio} parameterized semiempirical model that breaks electron-hole symmetry and nonequilibrium Green's function methods for the calculation of the conductance distribution $g$. The underlying mechanism is based on wavefunction localizations and perturbations that in the case of the first $\pi-\pi{}^*$ plateau can give rise to impurity-like pseudogaps with both donor and acceptor characteristics. Confinement and geometry are crucial for the manifestation of such effects. Self-consistent quantum transport calculations characterize vacancies as local charging centers that can induce electrostatic inhomogeneities on the ribbon topology., Comment: 5 pages, 4 figures, accepted for publication at PRB

We present electronic structure calculations of few-layer epitaxial graphene nanoribbons on SiC(0001). Trough an atomistic description of the graphene layers and the substrate within the extended H\"{u}ckel Theory and real/momentum space projections we argue that the role of the heterostructure's interface becomes crucial for the conducting capacity of the studied systems. The key issue arising from this interaction is a Fermi level pinning effect introduced by dangling interface bonds. Such phenomenon is independent from the width of the considered nanostructures, compromising the importance of confinement in these systems., Comment: 8 pages, 4 figures

Structure and electronic properties of two unusual boron clusters obtained by fusion of borozene rings has been studied by means of first principles calculations, based on the generalized-gradient approximation of the density functional theory, and the semiempirical tight-binding method was used for the transport calculations. The role of disorder has also been considered with single vacancies and substitutional atoms. Results show that the pure boron clusters are topologically planar and characterized by (3c-2e) bonds, which can explain, together with the aromaticity (estimated by means of NICS), the remarkable cohesive energy values obtained. Such feature makes these systems competitive with the most stable boron clusters to date. On the contrary, the introduction of impurities compromises stability and planarity in both cases. The energy gap values indicate that these clusters possess a semiconducting character, while when the larger system is considered, zero-values of the density of states are found exclusively within the HOMO-LUMO gap. Electron transport calculations within the Landauer formalism confirm these indications, showing semiconductor-like low bias differential conductance for these stuctures. Differences and similarities with Carbon clusters are highlighted in the discussion., Comment: 10 pages, 2 tables, 5 figures

A method for the study of the electronic transport in strongly coupled electron-phonon systems is formalized and applied to a model of polyyne chains biased through metallic Au leads. We derive a stationary non equilibrium polaronic theory in the general framework of a variational formulation. The numerical procedure we propose can be readily applied if the electron-phonon interaction in the device hamiltonian can be approximated as an effective single particle electron hamiltonian. Using this approach, we predict that finite polyyne chains should manifest an insulator-metal transition driven by the non-equilibrium charging which inhibits the Peierls instability characterizing the equilibrium state., Comment: to appear at EPJB

We implement a bottom-up multiscale approach for the modeling of defect localization in $C_{6n^2}H_{6n}$ islands, i.e. graphene quantum dots with a hexagonal symmetry, by means of density functional and semiempirical approaches. Using the \textit{ab initio} calculations as a reference, we recognize the theoretical framework under which semiempirical methods describe adequately the electronic structure of the studied systems and thereon proceed to the calculation of quantum transport within the non-equilibrium Green's function formalism. The computational data reveal an impurity-like behavior of vacancies in these clusters and evidence the role of parameterization even within the same semiempirical context. In terms of conduction, failure to capture the proper chemical aspects in the presence of generic local alterations of the ideal atomic structure results in an improper description of the transport features. As an example, we show wavefunction localization phenomena induced by the presence of vacancies and discuss the importance of their modeling for the conduction characteristics of the studied structures., Comment: 9 pages, 9 figures, accepted at J. Phys.: Condens. Matter