Atomic-Scale Moiré and Electronic Structure Analysis of Twisted Epitaxial MoS₂-Au-MoS₂ Heterostructures

Twisted epitaxy enables precise orientation control of nanostructures confined within van der Waals (vdW) gaps. Here, we investigate the moiré and electronic structure of a representative twisted epitaxial system, where Au nanodiscs are grown inside twisted bilayer MoS₂ with a 6° interlayer twist, inducing a 3° symmetrical misalignment of Au relative to each MoS₂ layer (MoS₂-Au-MoS₂). Using multislice electron ptychography (MEP), we resolve the three-dimensional "moiré-of-moirés" structure of MoS₂-Au-MoS₂ with atomic resolution. Electron energy loss spectroscopy (EELS) shows that MoS₂ encapsulation significantly reduces the plasmon energy of Au nanodiscs compared with their unencapsulated counterparts. Furthermore, first-principles calculations reveal that Au insertion alters the electronic band alignment near the Fermi level of bilayer MoS₂. Our results introduce a twisted MoS₂-Au-MoS₂ heterostructure as a structurally and electronically rich material system and establish twisted epitaxy as a new strategy for moiré engineering and the synthesis of 2D-confined materials with tunable optoelectronic properties.