Excitations of Intercalated Metal Monolayers in Transition Metal Dichalcogenides

We combine Raman scattering spectroscopy and lattice dynamics calculations to reveal the fundamental excitations of the intercalated metal monolayers in the FeTaS₂ (x = 1/4, 1/3) family of materials. Both in- and out-of-plane modes are identified, each of which has trends that depend upon the metal-metal distance, the size of the van der Waals gap, and the metal-to-chalcogenide slab mass ratio. We test these trends against the response of similar systems, including Cr-intercalated NbS₂ and RbFe(SO₄)₂, and demonstrate that the metal monolayer excitations are both coherent and tunable. We discuss the consequences of intercalated metal monolayer excitations for material properties and developing applications.