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Atomically thin GaSe has been predicted to have a non-parabolic, Mexican hat-like valence band structure due to the shift of the valence band maximum (VBM) near the Γ point which is expected to give rise to novel, unique properties such as tunable magnetism, high effective mass suppressing direct tunneling in scaled transistors, and an improved thermoelectric figure of merit. However, the synthesis of atomically thin GaSe remains challenging. Here, we report on the growth of atomically thin GaSe by molecular beam epitaxy (MBE) and demonstrate the high quality of the resulting van der Waals epitaxial films. The full valence band structure of nominal bilayer GaSe is revealed by photoemission electron momentum microscopy (k-PEEM), confirming the presence of a distorted valence band near the Γ point. Our results open the way to demonstrating interesting new physical phenomena based on MBE-grown GaSe films and atomically thin monochalcogenides in general.Molecular beam epitaxy: two-dimensional GaSe with non-parabolic electronic dispersionMolecular beam epitaxy enables growth of high-quality, atomically thin GaSe on a GaAs substrate. A team led by Andras Kis at EPFL successfully demonstrated the synthesis of large-grain GaSe van der Waals epitaxial films using a two-step growth approach. The quality and spatial uniformity of the as-grown films were probed by various means of characterization, including scanning transmission electron microscopy, in-situ reflection high energy electron diffraction, and photoemission electron momentum microscopy. The results indicate a uniform distribution of Ga and Se in the GaSe film; at the atomically thin limit, the electronic band structure was found to exhibit inverted band dispersion at the Γ point, leading to a Mexican Hat-like valence band dispersion. These finding may pave the way to potential applications of GaSe in large-area electronics and spintronics.

Large-grain MBE-grown GaSe on GaAs with a Mexican hat-like valence band dispersion