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.

17 pages (8 main, 9 SI)

References in corpus (27)

• Graphene plasmonics
• A real-space grid implementation of the Projector Augmented Wave method
• Quantum Plasmonics
• Hidden spin polarization in inversion-symmetric bulk crystals
• Direct observation of spin-polarised bulk bands in an inversion-symmetric semiconductor
• GPAW: An open Python package for electronic-structure calculations
• Spin-valley locking in the normal state of a transition-metal dichalocogenide superconductor
• Spontaneous topological Hall effect induced by non-coplanar antiferromagnetic order in intercalated van der Waals materials
• Uncovering and tailoring hidden Rashba spin-orbit splitting in centrosymmetric crystals
• Band structure engineered layered metals for low-loss plasmonics
• Collective Excitations in 2D Materials
• Tetrahedral triple-Q magnetic ordering and large spontaneous Hall conductivity in the metallic triangular antiferromagnet Co1/3TaS2
• The Effect of Charge Order on the Plasmon Dispersion in Transition-Metal Dichalcogenides
• Tailoring Dzyaloshinskii-Moriya interaction in a transition metal dichalcogenide by dual-intercalation
• Plasmons in the van der Waals charge-density-wave material 2H-TaSe2
• Orbital selectivity causing anisotropy and particle-hole asymmetry in the charge density wave gap of $2H$-TaS${}_2$
• Spectroscopic signature of the $\mathbf{k}$-dependent electron-phonon coupling in $2H$-TaS${}_2$
• Composition dependence of bulk properties in the Co-intercalated transition-metal dichalcogenide Co${}_{1/3}$TaS${}_2$
• Electron-energy-loss and time-dependent density functional theory study on the plasmon dispersion in 2H-NbS2
• Darkness in interlayer and charge density wave states of 2H-TaS2
• Slow, Nanometer Light Confinement Observed in Atomically Thin TaS2
• Intrinsic and extrinsic plasmons in the hard x-ray photoelectron spectra of nearly free electron metals
• Spin-Valley Locking in 2H-TaS2 and Its Co-Intercalated Counterpart: Roles of Surface Domains and Co Intercalation
• Ligand-mediated Origin of Altermagnetic Spin-Splitting
• Magnetoelastic coupling in intercalated transition metal dichalcogenides
• Electronic origin of delicate antiferromagnetism in Fe${}_x$NbS${}_2$
• An altermagnetic materials library in intercalated transition-metal dichalcogenides