Substrate pre-sputtering for layer-by-layer van der Waals epitaxy of 2D materials

Two-dimensional transition metal chalcogenides, with their atomically layered structure, favourable electronic and mechanical properties, and often strong spin-orbit coupling, are ideal systems for fundamental studies and for applications ranging from spintronics to optoelectronics. Their bottom-up synthesis via epitaxial techniques such as molecular-beam epitaxy (MBE) has, however, proved challenging. Here, we develop a simple substrate pre-treatment process utilising exposure to a low-energy noble gas plasma. We show how this dramatically enhances nucleation of an MBE-grown epilayer atop, and through this, realise a true layer-by-layer growth mode. We further demonstrate the possibility of tuning the resulting growth dynamics via control of the species and dose of the plasma exposure.