On the van der Waals Epitaxy of Homo-/Heterostructures of Transition Metal Dichalcogenides

Layered materials held together by weak van der Waals (vdW) interactions are a promising class of materials in the field of nanotechnology. Besides the potential for single layers, stacking of various vdW layers becomes even more promising since unique properties can hence be precisely engineered. The synthesis of stacked vdW layers, however, remains to date, hardly understood. Therefore, in this work, the vdW epitaxy of transition metal dichalcogenides (TMDs) on single-crystalline TMD templates is investigated in depth. It is demonstrated that the role of lattice mismatch is insignificant. More importantly is the role of surface energy, calculated using density functional theory, which plays an essential role in the activation energy for adatom diffusion, hence nucleation density. This in turn correlates with defect density since the stacking sequence in vdW epitaxy is generally poorly controlled. Moreover, the vapor pressure of the transition metal is also found to correlate with adatom diffusion. Consequently, the proposed study enables important and new insight in the vdW epitaxy of multilayer 2D homo-/heterostructures.