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Theory of liquid film growth and wetting instabilities on graphene

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 Added by Adrian Del Maestro
 Publication date 2017
  fields Physics
and research's language is English




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We investigate wetting phenomena near graphene within the Dzyaloshinskii-Lifshitz-Pitaevskii theory for light gases composed of hydrogen, helium and nitrogen in three different geometries where graphene is either affixed to an insulating substrate, submerged or suspended. We find that the presence of graphene has a significant effect in all configurations. In a suspended geometry where graphene is able to wet on only one side, liquid film growth becomes arrested at a critical thickness which may trigger surface instabilities and pattern formation analogous to spinodal dewetting. These phenomena are also universally present in other two-dimensional materials.



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We demonstrate theoretically the possibility of spinodal de-wetting in heterostructures made of light--atom liquids (hydrogen, helium, and nitrogen) deposited on suspended graphene. Extending our theory of film growth on two-dimensional materials to include analysis of surface instabilities via the hydrodynamic Cahn--Hilliard-type equation, we characterize in detail the resulting spinodal de-wetting patterns. Both linear stability analysis and advanced computational treatment of the surface hydrodynamics show micron-sized (generally material and atom dependent) patterns of dry regions. The physical reason for the development of such instabilities on graphene can be traced back to the inherently weak van der Waals interactions between atomically thin materials and atoms in the liquid. Similar phenomena occur in doped graphene and other two-dimensional materials, such as monolayer dichalcogenides. Thus two-dimensional materials represent a universal theoretical and technological platform for studies of spinodal de-wetting.
Tellurium (Te) films with monolayer and few-layer thickness are obtained by molecular beam epitaxy on a graphene/6H-SiC(0001) substrate and investigated by in situ scanning tunneling microscopy and spectroscopy (STM/STS). We reveal that the Te films are composed of parallel-arranged helical Te chains flat-lying on the graphene surface, exposing the (1x1) facet of (10-10) of the bulk crystal. The band gap of Te films increases monotonically with decreasing thickness, reaching ~0.92 eV for the monolayer Te. An explicit band bending at the edge between the monolayer Te and graphene substrate is visualized. With the thickness controlled in atomic scale, Te films show potential applications of in electronics and optoelectronics.
The interaction of interfacial water with graphitic carbon at the atomic scale is studied as a function of the hydrophobicity of epitaxial graphene. High resolution X-ray reflectivity shows that the graphene-water contact angle is controlled by the average graphene thickness, due to the fraction of the film surface expressed as the epitaxial buffer layer whose contact angle (contact angle theta_c = 73{deg}) is substantially smaller than that of multilayer graphene (theta_c = 93{deg}). Classical and ab initio molecular dynamics simulations show that the reduced contact angle of the buffer layer is due to both its epitaxy with the SiC substrate and the presence of interfacial defects. This insight clarifies the relationship between interfacial water structure and hydrophobicity, in general, and suggests new routes to control interface properties of epitaxial graphene.
We demonstrate molecular beam growth of graphene on biotite mica substrates at temperatures below 1000{deg}C. As indicated by optical and atomic force microscopy, evaporation of carbon from a high purity solid-state source onto biotite surface results in the formation of single-, bi-, and multilayer graphene with size in the micrometer regime. Graphene grown directly on mica surface is of very high crystalline quality with the defect density below the threshold detectable by Raman spectroscopy. The interaction between graphene and the mica substrate is studied by comparison of the Raman spectroscopy and atomic force microscopy data with the corresponding results obtained for graphene flakes mechanically exfoliated onto biotite substrates. Experimental insights are combined with density functional theory calculations to propose a model for the initial stage of the van der Waals growth of graphene on mica surfaces. This work provides important hints on how the direct growth of high quality graphene on insulators can be realized in general without exceeding the thermal budget limitations of Si technologies.
In this paper, the interfacial motion between two immiscible viscous fluids in the confined geometry of a Hele-Shaw cell is studied. We consider the influence of a thin wetting film trailing behind the displaced fluid, which dynamically affects the pressure drop at the fluid-fluid interface by introducing a nonlinear dependence on the interfacial velocity. In this framework, two cases of interest are analyzed: The injection-driven flow (expanding evolution), and the lifting plate flow (shrinking evolution). In particular, we investigate the possibility of controlling the development of fingering instabilities in these two different Hele-Shaw setups when wetting effects are taken into account. By employing linear stability theory, we find the proper time-dependent injection rate $Q(t)$ and the time-dependent lifting speed ${dot b}(t)$ required to control the number of emerging fingers during the expanding and shrinking evolution, respectively. Our results indicate that the consideration of wetting leads to an increase in the magnitude of $Q(t)$ [and ${dot b}(t)$] in comparison to the non-wetting strategy. Moreover, a spectrally accurate boundary integral approach is utilized to examine the validity and effectiveness of the controlling protocols at the fully nonlinear regime of the dynamics and confirms that the proposed injection and lifting schemes are feasible strategies to prescribe the morphologies of the resulting patterns in the presence of the wetting film.
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