Plasmon Engineering in Intercalated 2H-TaS$_2$

Abstract

Plasmons in low dimensional materials provide a powerful platform for nanoscale control of light matter interactions, yet strategies to tailor their coherence and dissipation remain limited. Here, we demonstrate that transition metal intercalation offers a fundamentally distinct route to engineer plasmonic response in layered materials. By combining high-resolution core-level photoemission spectroscopy with first-principles calculations, we show that Fe and Co intercalation in 2H-TaS2 does not act as conventional electron doping, but instead reshapes the low energy electronic structure through orbital hybridization and structural reconstruction. This process introduces a dense continuum of low energy excitations that efficiently damp and ultimately suppress the plasmon mode. First principle calculations of the energy loss function reveal a transition from a well defined collective excitation to an overdamped response, signaling the breakdown of coherent charge dynamics. Our results establish intercalation as a chemically controlled pathway to tune plasmon losses and dielectric response in quantum van der Waals materials, providing a new design principle for plasmonic and optoelectronic functionalities at the nanoscale.