Zerovalent-Metal Intercalated MoS₂ Hybrids for Optoelectronics

The intercalation of layered compounds is a promising route for scalable synthesis of 2D heterostructures with novel emergent optoelectronic properties. Here, we investigate, via first principles calculations, the intercalation of zerovalent metals within the van der Waals gap of bulk MoS₂. Specifically, we focus on Cu-MoS₂ and Sn-MoS₂hybrids that can accommodate Cu and Sn, ranging from clusters to continuous 2D layers within the vdW gap of MoS₂. We study the evolution of the Cu-MoS₂ and Sn-MoS₂ hybrids with increasing metal content and examine the consequences for intercalation energetics and optoelectronic properties as the intercalated metals evolve from disordered clusters to contiguous layers. We identify emergent interfacial plasmons (1-2 eV range) that are unique to these intercalated materials, arising from resonant 2D metallic states within the MoS₂ band gap. Our calculations are shown to be in good agreement with experiments and help explain the enhanced infrared absorption of the Cu-MoS₂ and Sn-MoS₂ hybrids. Overall, our results indicate that intercalation of zerovalent metals in layered materials offers a facile and scalable approach for designing hybrid 2D heterostructures with tunable optoelectronic properties for device applications.