Tripling of the scattering vector range of X-ray reflectivity on liquid surfaces using a double-crystal deflector.

The maximum range of perpendicular momentum transfer ( ) has been tripled for X-ray scattering from liquid surfaces when using a double-crystal deflector setup to tilt the incident X-ray beam. This is achieved by employing a higher-energy X-ray beam to access Miller indices of reflecting crystal atomic planes that are three times higher than usual. The deviation from the exact Bragg angle condition induced by misalignment between the X-ray beam axis and the main rotation axis of the double-crystal deflector is calculated, and a fast and straightforward procedure to align them is deduced.

Superstructures, Commensurations, and Rotation of Single-Layer TaS on Au(111) Induced by Cs Intercalation/Deintercalation.

We use synchrotron grazing incidence X-ray diffraction and X-ray reflectivity to investigate with high resolution the structure of a two-dimensional single layer of tantalum sulfide grown on a Au(111) surface and its evolution during intercalation by Cs atoms and deintercalation, which decouples and recouples the two materials, respectively. The grown single layer consists of a mixture of TaS and its S-depleted version, TaS, both aligned with gold, and forming moirés where 7 (respectively 13) lattice constants of the 2D layer almost perfectly match 8 (respectively 15) substrate lattice constants. Intercalation fully decouples the system by lifting the single layer by ∼370 pm and induces an increase of its lattice parameter by 1-2 picometers.

Graphene at Liquid Copper Catalysts: Atomic-Scale Agreement of Experimental and First-Principles Adsorption Height.

Liquid metal catalysts have recently attracted attention for synthesizing high-quality 2D materials facilitated via the catalysts' perfectly smooth surface. However, the microscopic catalytic processes occurring at the surface are still largely unclear because liquid metals escape the accessibility of traditional experimental and computational surface science approaches. Hence, numerous controversies are found regarding different applications, with graphene (Gr) growth on liquid copper (Cu) as a prominent prototype.

X-ray reflectivity from curved surfaces as illustrated by a graphene layer on molten copper.

The X-ray reflectivity technique can provide out-of-plane electron-density profiles of surfaces, interfaces, and thin films, with atomic resolution accuracy. While current methodologies require high surface flatness, this becomes challenging for naturally curved surfaces, particularly for liquid metals, due to the very high surface tension. Here, the development of X-ray reflectivity measurements with beam sizes of a few tens of micrometres on highly curved liquid surfaces using a synchrotron diffractometer equipped with a double crystal beam deflector is presented.

Real-Time Multiscale Monitoring and Tailoring of Graphene Growth on Liquid Copper.

The synthesis of large, defect-free two-dimensional materials (2DMs) such as graphene is a major challenge toward industrial applications. Chemical vapor deposition (CVD) on liquid metal catalysts (LMCats) is a recently developed process for the fast synthesis of high-quality single crystals of 2DMs. However, up to now, the lack of techniques enabling direct feedback on the growth has limited our understanding of the process dynamics and primarily led to empirical growth recipes.

Elaboration of Nanomagnet Arrays: Organization and Magnetic Properties of Mass-Selected FePt Nanoparticles Deposited on Epitaxially Grown Graphene on Ir(111).

The moiré pattern created by the epitaxy of a graphene sheet on an iridium substrate can be used as a template for the growth of 2D atomic or cluster arrays. We observed for the first time a coherent organization of hard magnetic preformed FePt nanoparticles on the 2D lattice of graphene on Ir(111). Nanoparticles of 2 nm diameter have been mass selected in a gas phase and deposited with low energy on the hexagonal moiré pattern.

Beyond van der Waals Interaction: The Case of MoSe 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 MoSe/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.

Massless Dirac Fermions in ZrTe Semimetal Grown on InAs(111) by van der Waals Epitaxy.

Single and few layers of the two-dimensional (2D) semimetal ZrTe are grown by molecular beam epitaxy on InAs(111)/Si(111) substrates. Excellent rotational commensurability, van der Waals gap at the interface and moiré pattern are observed indicating good registry between the ZrTe epilayer and the substrate through weak van der Waals forces. The electronic band structure imaged by angle resolved photoelectron spectroscopy shows that valence and conduction bands cross at the Fermi level exhibiting abrupt linear dispersions.

Moiré induced organization of size-selected Pt clusters soft landed on epitaxial graphene.

Two-dimensional hexagonal arrays of Pt nanoparticles (1.5 nm diameter) have been obtained by deposition of preformed and size selected Pt nanoparticles on graphene. This original self-organization is induced, at room temperature, by the 2D periodic undulation (the moiré pattern) of graphene epitaxially grown on the Ir(111) surface.

Strains induced by point defects in graphene on a metal.

Strains strongly affect the properties of low-dimensional materials, such as graphene. By combining in situ, in operando, reflection high-energy electron diffraction experiments with first-principles calculations, we show that large strains, above 2%, are present in graphene during its growth by chemical vapor deposition on Ir(111) and when it is subjected to oxygen etching and ion bombardment. Our results unravel the microscopic relationship between point defects and strains in epitaxial graphene and suggest new avenues for graphene nanostructuring and engineering its properties through introduction of defects and intercalation of atoms and molecules between graphene and its metal substrate.

Effects of near-neighbor correlations on the diffuse scattering from a one-dimensional paracrystal.

The one-dimensional paracrystal model is generalized by folding the lattice sites with objects whose scattering lengths or sizes and separation display a spatial correlation from cell to cell. A general theory to calculate the diffuse scattering and the scattering-length autocorrelation function is developed. The investigated models of coupling along the paracrystalline chain are the correlations between (i) the sizes of the scatterers, (ii) the sizes of scatterers and their separations, and (iii) the sizes of scatterers and the fluctuation of their separation distances.

Real-time monitoring of growing nanoparticles.

One challenge in the production of nanometer-sized objects with given properties is to control their growth at a macroscopic scale in situ and in real time. A dedicated ultrahigh-vacuum grazing-incidence small-angle x-ray scattering setup has been developed, yielding high sensitivity and dynamics. Its capabilities to derive the average particle shape and size and the film growth mode and ordering and to probe both surfaces and buried interfaces are illustrated for two prototypical cases: the model catalyst Pd/MgO(100) and the self-organized Co/Au(111) system.