Aurélien Lherbier

Damaging Graphene with ozone treatment : a chemically tunable metal-insulator transition

We present a multiscale ab initio study of electronic and transport properties of two-dimensional graphene after epoxide functionalization via ozone treatment. The orbital rehybridization induced by the epoxide groups triggers a strong intervalley scattering and changes dramatically the conduction properties of graphene. By varying the coverage density of epoxide defects from 0.1 to 4%, charge conduction can be tuned from a diffusive to a strongly localized regime, with localization lengths down to a few nanometers long. Experimental results supporting the interpretation as a metal-insulator transition are also provided.

Transport Length Scales in Disordered Graphene-based Materials: Strong Localization Regimes and Dimensionality Effects

We report on a numerical study of quantum transport in disordered two dimensional graphene and graphene nanoribbons. By using the Kubo and the Landauer approaches, transport length scales in the diffusive (mean free path and charge mobilities) and localized regimes (localization lengths) are computed, assuming a short range disorder (Anderson-type). The electronic systems are found to undergo a conventional Anderson localization in the zero-temperature limit, in agreement with localization scaling theory. Localization lengths in weakly disordered ribbons are found to strongly fluctuate depending on their edge symmetry, but always remain several orders of magnitude smaller than those computed for 2D graphene for the same disorder strength. This pinpoints the role of transport dimensionality and edge effects.

Transport properties of graphene containing structural defects

We propose an extensive report on the simulation of electronic transport in two-dimensional graphene in presence of structural defects. Amongst the large variety of such defects in sp2 carbon-based materials, we focus on the Stone-Wales defect and on two divacancy-type reconstructed defects. Based on ab initio calculations, a tight-binding model is derived to describe the electronic structure of these defects. Semiclassical transport properties including the elastic mean-free paths, mobilities, and conductivities are computed using an order-N real-space Kubo-Greenwood method. A plateau of minimum conductivity (σmin sc = 4e2/πh) is progressively observed as the density of defects increases. This saturation of the decay of conductivity to σmin sc is associated with defect-dependent resonance energies. Finally, localization phenomena are captured beyond the semiclassical regime. An Anderson transition is predicted with localization lengths of the order of tens of nanometers for defect densities around 1%.

Electronic and transport properties of unbalanced sublattice N-doping in graphene

Using both first-principles techniques and a real-space Kubo-Greenwood approach, electronic and transport properties of nitrogen-doped graphene with a single sublattice preference are investigated. Such a breaking of the sublattice symmetry leads to the appearance of a true band gap in graphene electronic spectrum even for a random distribution of the N dopants. More surprisingly, a natural spatial separation of both types of charge carriers at the band edge is predicted, leading to a highly asymmetric electronic transport. Both the presence of a band gap, allowing large on/off ratio, and an asymmetric transport pave a new route toward efficient graphene-based field-effect transistors.

Two-Dimensional Graphene with Structural Defects: Elastic Mean Free Path, Minimum Conductivity, and Anderson Transition

Quantum transport properties of disordered graphene with structural defects (Stone-Wales and divacancies) are investigated using a realistic π-π* tight-binding model elaborated from ab initio calculations. Mean free paths and semiclassical conductivities are then computed as a function of the nature and density of defects (using an order-N real-space Kubo-Greenwood method). By increasing the defect density, the decay of the semiclassical conductivities is predicted to saturate to a minimum value of 4e2/πh over a large range (plateau) of carrier density (>0.5×10(14)  cm(-20). Additionally, strong contributions of quantum interferences suggest that the Anderson localization regime could be experimentally measurable for a defect density as low as 1%.

Orientational Dependence of Charge Transport in Disordered Silicon Nanowires

We report on a theoretical study of surface roughness effects on charge transport in silicon nanowires with three different crystalline orientations, [100], [110] and [111]. Using an atomistic tight-binding model, key transport features such as mean-free paths, charge mobilities, and conductance scaling are investigated with the complementary Kubo-Greenwood and Landauer-Büttiker approaches. The anisotropy of the band structure of bulk silicon results in a strong orientation dependence of the transport properties of the nanowires. The best orientations for electron and hole transport are found to be the [110] and [111] directions, respectively.

Quantum transport in chemically modified two-dimensional graphene: From minimal conductivity to Anderson localization

An efficient computational methodology is used to explore charge transport properties in chemically modified (and randomly disordered) graphene-based materials. The Hamiltonians of various complex forms of graphene are constructed using tight-binding models enriched by first-principles calculations. These atomistic models are further implemented into a real-space order-N Kubo-Greenwood approach, giving access to the main transport length scales (mean free paths, localization lengths) as a function of defect density and charge carrier energy. An extensive investigation is performed for epoxide impurities with specific discussions on both the existence of a minimum semiclassical conductivity and a crossover between weak to strong localization regime. The 2D generalization of the Thouless relationship linking transport length scales is here illustrated based on a realistic disorder model.

Quantum Transport Length Scales in Silicon-based Semiconducting Nanowires: Surface Roughness Effects

We report on a theoretical study of quantum charge transport in atomistic models of silicon nanowires with surface roughness disorder, using an efficient real-space, order N Kubo-Greenwood approach and a Landauer-Buttiker Greens function method. Different transport regimes (from quasiballistic to localization) are explored depending on the length of the nanowire and the characteristics of the surface roughness profile. Quantitative estimates of the elastic mean free paths, charge mobilities, and localization lengths are provided as a function of the correlation length of the surface roughness disorder. Moreover, the limitations of the Thouless relation between the mean free path and the localization length are outlined.

Band widths and gaps from the Tran-Blaha functional: Comparison with many-body perturbation theory

For a set of ten crystalline materials (oxides and semiconductors), we compute the electronic band structures using the Tran-Blaha (TB09) functional. The band widths and gaps are compared with those from the local-density approximation (LDA) functional, many-body perturbation theory (MBPT), and experiments. At the density-functional theory (DFT) level, TB09 leads to band gaps in much better agreement with experiments than LDA. However, we observe that it globally underestimates, often strongly, the valence (and conduction) band widths (more than LDA). MBPT corrections are calculated starting from both LDA and TB09 eigenenergies and wave functions. They lead to a much better agreement with experimental data for band widths. The band gaps obtained starting from TB09 are close to those from quasiparticle self-consistent GW calculations, at a much reduced cost. Finally, we explore the possibility to tune one of the semiempirical parameters of the TB09 functional in order to obtain simultaneously better band gaps and widths. We find that these requirements are conflicting.

Electronic and optical properties of pristine and oxidized borophene

Borophene, a two-dimensional monolayer of boron atoms, was recently synthesized experimentally and was shown to exhibit polymorphism. In its closed-packed triangular form, borophene is expected to exhibit anisotropic metallic character with relatively high electron velocities. At the same time, very low optical conductivities in the infrared-visible light region were predicted. Based on its promising electronic transport properties and its high transparency, borophene could become a genuine lego piece in the 2D materials assembling game known as the van der Waals heterocrystal approach. However, borophene is naturally degraded in ambient conditions and it is therefore important to assess the mechanisms and the effects of oxidation on borophene monolayers. Optical and electronic properties of pristine and oxidized borophene are here investigated by first-principles approaches. The transparent and conductive properties of borophene are elucidated by analyzing the electronic structure and its interplay with light. Optical response of borophene is found to be strongly affected by oxidation, suggesting that optical measurements can serve as an efficient probe for borophene surface contamination.