Plasmon properties and hybridization effects in Silicene

TL;DR

This paper investigates the plasmonic properties of monolayer silicene using time-dependent density functional theory, revealing intrinsic interband modes, extrinsic intraband modes, and their dependence on charge doping and lattice structure.

Contribution

It provides a detailed analysis of silicene's plasmon resonances, including hybridized and conventional modes, and highlights their sensitivity to doping and lattice effects, expanding understanding beyond graphene.

Findings

Identification of hybridized pi-like and pi-sigma plasmons above 1.5 eV.

Prediction of extrinsic intraband modes, including a 2D and an acoustic plasmon.

Plasmons are highly sensitive to charge doping and lattice structure, independent of chemistry.

Abstract

The plasmonic character of monolayer silicene is investigated by time-dependent density functional theory in the random phase approximation. The energy-loss function of the system is analyzed, with particular reference to its induced charge-density fluctuations, i.e., plasmon resonances and corresponding dispersions, occurring in the investigated energy-momentum region. At energies larger than 1.5eV, two intrinsic interband modes are detected and characterized. The first one is a hybridized pi-like plasmon, which is assisted by competing one-electron processes involving sp2 and sp3 states. The second one is a more conventional pi-sigma plasmon, which is more intense than the pi-like plasmon and more affected by one-electron processes involving the sigma bands, with respect to the analogous collective oscillation in monolayer graphene. At energies below 1eV, two extrinsic intraband modes are predicted to occur, which are generated by distinct types of Dirac electrons (associated with different Fermi velocities at the so-called Dirac points). The most intense of them is a two-dimensional plasmon, having an energy-momentum dispersion that resembles that of a two-dimensional electron gas. The other is an acoustic plasmon that occurs for specific momentum directions and competes with the two-dimensional plasmon at mid infrared energies. The strong anisotropic character of this mode cannot be explained in terms of the widely used Dirac-cone approximation. As in mono-, bi-, and few-layer graphene, the extrinsic oscillations of silicene are highly sensitive to the concentration of injected or ejected charge carriers. More importantly, the two-dimensional and acoustic plasmons appear to be a signature of the honeycomb lattice, independently of the chemistry of the group-IV elements and the details of the unit-cell geometry.