Observation of Gap Opening in 1T' Phase MoS₂ Nanocrystals

Two-dimensional (2D) transition metal dichalcogenides (TMDs) manifest in various polymorphs, which deliver different electronic properties; the most prominent among them include the semiconducting 2H phase and metallic 1T (or distorted 1T' phase) phase. Alkali metal intercalation or interface strain has been used to induce semiconductor-to-metal transition in a monolayer MoS₂ sheet, leading to exotic quantum states or improved performance in catalysis. However, the direct growth of 1T or 1T' phase MoS₂ is challenging due to its metastability. Here, we report MBE growth of isolated 1T' and 2H MoS₂ nanocrystals on a Au substrate; these nanocrystals can be differentiated unambiguously by their electronic states using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). By studying the initial stages of nucleation during molecular beam epitaxy (MBE) of MoS₂, we could identify atomic clusters (30-50 atoms) with intralayer stacking corresponding to 1T' and 2H separately, which suggests a deterministic growth mechanism from initial nuclei. Furthermore, a topological insulator type behavior was observed for the 1T' MoS₂ crystals, where an energy gap opening of 80 meV was measured by STS in the basal plane at 5 K, with the edge of the nanocrystals remaining metallic.