Heterostrain Determines Flat Bands in Magic-Angle Twisted Graphene Layers.

The moiré of twisted graphene bilayers can generate flat bands in which charge carriers do not possess enough kinetic energy to escape Coulomb interactions with each other, leading to the formation of novel strongly correlated electronic states. This exceptionally rich physics relies on the precise arrangement between the layers. Here, we survey published scanning tunneling microscope measurements to prove that near the magic-angle, native heterostrain, the relative deformations between the layers, dominates twist in determining the flat bands as opposed to the common belief. This is demonstrated at full filling where electronic correlations have a weak effect and where we also show that tip-induced strain can have a strong influence. In the opposite situation of zero doping, we find that electronic correlation further renormalizes the flat bands in a way that strongly depends on experimental details.

Size-Selective Carbon Clusters as Obstacles to Graphene Growth on a Metal.

Chemical vapor deposition (CVD) on metals is so far the best suited method to produce high-quality, large-area graphene. We discovered an unprecedentedly large family of small size-selective carbon clusters that form together with graphene during CVD. Using scanning tunneling microscopy (STM) and density functional theory (DFT), we unambiguously determine their atomic structure. For that purpose, we use grids based on a graphene moiré and a dilute atomic lattice that unambiguously reveal the binding geometry of the clusters. We find that the observed clusters bind in metastable configurations on the substrate, while the thermodynamically stable configurations are not observed. We argue that the clusters are formed under kinetic control and establish that the evolution of the smallest clusters is blocked. They are hence products of surface reactions in competition with graphene growth, rather than intermediary species to the formation of extended graphene, as often assumed in the literature. We expect such obstacles to the synthesis of perfect graphene to be ubiquitous on a variety of metallic surfaces.

Electronic Spectrum of Twisted Graphene Layers under Heterostrain.

We demonstrate that stacking layered materials allows a strain engineering where each layer is strained independently, which we call heterostrain. We combine detailed structural and spectroscopic measurements with tight-binding calculations to show that small uniaxial heterostrain suppresses Dirac cones and leads to the emergence of flat bands in twisted graphene layers (TGLs). Moreover, we demonstrate that heterostrain reconstructs, much more severely, the energy spectrum of TGLs than homostrain for which both layers are strained identically, a result which should apply to virtually all van der Waals structures opening exciting possibilities for straintronics with 2D materials.

Giant Atomic Swirl in Graphene Bilayers with Biaxial Heterostrain.

The study of moiré engineering started with the advent of van der Waals heterostructures, in which stacking 2D layers with different lattice constants leads to a moiré pattern controlling their electronic properties. The field entered a new era when it was found that adjusting the twist between two graphene layers led to strongly-correlated-electron physics and topological effects associated with atomic relaxation. A twist is now routinely used to adjust the properties of 2D materials. This study investigates a new type of moiré superlattice in bilayer graphene when one layer is biaxially strained with respect to the other-so-called biaxial heterostrain. Scanning tunneling microscopy measurements uncover spiraling electronic states associated with a novel symmetry-breaking atomic reconstruction at small biaxial heterostrain. Atomistic calculations using experimental parameters as inputs reveal that a giant atomic swirl forms around regions of aligned stacking to reduce the mechanical energy of the bilayer. Tight-binding calculations performed on the relaxed structure show that the observed electronic states decorate spiraling domain wall solitons as required by topology. This study establishes biaxial heterostrain as an important parameter to be harnessed for the next step of moiré engineering in van der Waals multilayers.

Superconducting group-IV semiconductors.

Despite the amount of experimental and theoretical work on doping-induced superconductivity in covalent semiconductors based on group IV elements over the past four years, many open questions and puzzling results remain to be clarified. The nature of the coupling (whether mediated by electronic correlation, phonons or both), the relationship between the doping concentration and the critical temperature (T(c)), which affects the prospects for higher transition temperatures, and the influence of disorder and dopant homogeneity are debated issues that will determine the future of the field. Here, we present recent achievements and predictions, with a focus on boron-doped diamond and silicon. We also suggest that innovative superconducting devices, combining specific properties of diamond or silicon with the maturity of semiconductor-based technologies, will soon be developed.

Elementary processes governing V2AlC chemical etching in HF.

The literature on MXenes, an important class of 2D materials discovered in 2011, is now abundant. Yet, the lack of well-defined structures, with definite crystal orientations, has so far hindered our capability to identify some key aspects ruling MXene's chemical exfoliation from their parent MAX phase. Herein the chemical exfoliation of V2AlC is studied by using well-defined square pillars with lateral sizes from 7 µm up to 500 µm, processed from centimeter-sized V2AlC single crystals. The MXene conversion kinetics are assessed with µm spatial resolution by combining Raman spectroscopy with scanning electron and optical microscopies. HF penetration, and the loss of the Al species, take place through the edges. At room temperature, and on a reasonable time scale, no etching can takes place by HF penetration through the basal planes, viz. normal to the basal planes. In defect-free pillars, etching through the edges is isotropic. Initially the etching rate is linear with a rate of 2.2 ± 0.3 µm h-1 at 25 °C. At a distance of ≈45 µm, the etching rate is greatly diminished.

Graphene as a Mechanically Active, Deformable Two-Dimensional Surfactant.

In crystal growth, surfactants are additive molecules used in dilute amount or as dense, permeable layers to control surface morphologies. We investigate the properties of a strikingly different surfactant: a 2D and covalent layer with close atomic packing, graphene. Using in situ, real-time electron microscopy, scanning tunneling microscopy, kinetic Monte Carlo simulations, and continuum mechanics calculations, we reveal why metallic atomic layers can grow in a 2D manner below an impermeable graphene membrane. Upon metal growth, graphene dynamically opens nanochannels called wrinkles, facilitating mass transport while at the same time storing and releasing elastic energy via lattice distortions. Graphene thus behaves as a mechanically active, deformable surfactant. The wrinkle-driven mass transport of the metallic layer intercalated between graphene and the substrate is observed for two graphene-based systems, characterized by different physicochemical interactions, between graphene and the substrate and between the intercalated material and graphene. The deformable surfactant character of graphene that we unveil should then apply to a broad variety of species, opening new avenues for using graphene as a 2D surfactant forcing the growth of flat films, nanostructures, and unconventional crystalline phases.

Beyond van der Waals Interaction: The Case of MoSe2 Epitaxially Grown on Few-Layer Graphene.

Van der Waals heterojunctions composed of graphene and transition metal dichalcogenides have gain much attention because of the possibility to control and tailor band structure, promising applications in two-dimensional optoelectronics and electronics. In this report, we characterized the van der Waals heterojunction MoSe2/few-layer graphene with a high-quality interface using cutting-edge surface techniques scaling from atomic to microscopic range. These surface analyses gave us a complete picture of the atomic structure and electronic properties of the heterojunction. In particular, we found two important results: the commensurability between the MoSe2 and few-layer graphene lattices and a band-gap opening in the few-layer graphene. The band gap is as large as 250 meV, and we ascribed it to an interface charge transfer that results in an electronic depletion in the few-layer graphene. This conclusion is well supported by electron spectroscopy data and density functional theory calculations. The commensurability between the MoSe2 and graphene lattices as well as the band-gap opening clearly show that the interlayer interaction goes beyond the simple van der Waals interaction. Hence, stacking two-dimensional materials in van der Waals heterojunctions enables us to tailor the atomic and electronic properties of individual layers. It also permits the introduction of a band gap in few-layer graphene by interface charge transfer.

Electric field-controlled rippling of graphene.

Metal-graphene interfaces generated by electrode deposition induce barriers or potential modulations influencing the electronic transport properties of graphene based devices. However, their impact on the local mechanical properties of graphene is much less studied. Here we show that graphene near a metallic interface can exhibit a set of ripples self-organized into domains whose topographic roughness is controlled by the tip bias of a scanning tunneling microscope. The reconstruction from topographic images of graphene bending energy maps sheds light on the local electro-mechanical response of graphene under STM imaging and unveils the role of the stress induced by the vicinity of the graphene-metal interface in the formation and the manipulation of these ripples. Since microscopic rippling is one of the important factors that limit charge carrier mobility in graphene, the control of rippling with a gate voltage may have important consequences in the conductance of graphene devices where transverse electric fields are created by contactless suspended gate electrodes. This opens up also the possibility to dynamically control the local morphology of graphene nanomembranes.

Pseudogap in a thin film of a conventional superconductor.

A superconducting state is characterized by the gap in the electronic density of states, which vanishes at the superconducting transition temperature T(c). It was discovered that in high-temperature superconductors, a noticeable depression in the density of states, the pseudogap, still remains even at temperatures above T(c). Here, we show that a pseudogap exists in a conventional superconductor, ultrathin titanium nitride films, over a wide range of temperatures above T(c). Our study reveals that this pseudogap state is induced by superconducting fluctuations and favoured by two-dimensionality and by the proximity to the transition to the insulating state. A general character of the observed phenomenon provides a powerful tool to discriminate between fluctuations as the origin of the pseudogap state and other contributions in the layered high-temperature superconductor compounds.