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Van der Waals (vdW) epitaxial growth of large-area and stable two-dimensional (2D) materials of high structural quality on crystalline substrates is crucial for the development of novel device technologies. 2D gallium monochalcogenides with low in-plane symmetry stand out among the layered semiconductor materials family for next-generation optoelectronic and energy conversion applications. Here, we demonstrate the formation of large-area, single crystal and optically active 2D monoclinic gallium telluride (m-GaTe) on silicon substrate via rapid thermal annealing induced phase transformation of vdW epitaxial metastable hexagonal gallium telluride (h-GaTe). Stabilization of multilayer h-GaTe on Si occurs due to the role of the first layer symmetry together with efficient GaTe surface passivation. Moreover, we show that the phase transformation of h-GaTe to m-GaTe is accompanied by the strain relaxation between Si substrate and GaTe. This work opens the way to the fabrication of single-crystal 2D anisotropic semiconductors on standard crystalline wafers that are difficult to be obtained by epitaxial methods.

Islands in the form of truncated triangular pyramids on the surface of an epitaxial Ge3Sb2Te6 layer grown on a Si(111) substrate are identified by scanning electron microscopy. It is established that sides of their bases are oriented along the Si〈110〉 directions, and sizes vary from several tens to several hundred nanometers. It is shown by high-resolution electron microscopy of cross-sectional specimens that the (111) planes of the cubic phase or (0001) planes of the hexagonal phase of Ge3Sb2Te6 in the epitaxial layer are oriented parallel to Si(111) and, in surface domains, can make an angle of 70.5° with the layer–substrate interface. It is established, using an atomic structure analysis and energy-dispersive X-ray microanalysis, that the composition in islands changes from Ge3Sb2Te6 to GeSb2Te4 along the growth direction.

GeSbTe (GST) phase-change alloys feature layered crystalline structures made of lamellae separated by van der Waals (vdW) gaps. This work sheds light on the dependence of interlamellae interactions at the vdW gap on film thickness of GST alloys as probed by vibrational spectroscopy. Molecular beam epitaxy is used for designing GST layers down to a single lamella. By combining density-functional theory and Raman spectroscopy, a direct and simple method is demonstrated to identify the thickness of the GST film. The shift of the vibrational modes is studied as a function of the layer size, and the low-frequency range opens up a new route to probe the number of lamellae for different GST compositions. Comparison between experimental and theoretical Raman spectra highlights the precision growth control obtained by the epitaxial technique.

Molecular dynamics based on the empirical Tersoff potential was used to simulate the deposition of amorphous silicon and germanium on silicon(111) at various deposition rates and temperatures. The resulting films were analyzed quantitatively by comparing one-dimensional atomic density profiles to experimental measurements. It is found that the simulations are able to capture well the structural features of the deposited films, which exhibit a gradual loss of crystalline order over several monolayers. A simple mechanistic model is used to demonstrate that the simulation temperature may be used to effectively accelerate the surface relaxation processes during deposition, leading to films that are consistent with experimental samples grown at deposition rates many orders-of-magnitude slower than possible in a molecular dynamics simulation.