Chemically doped graphene could support plasmon excitations up to telecommunication or even visible frequencies. Apart from that, the presence of dopant may influence electron scattering mechanisms in graphene and thus impact the plasmon decay rate. Here I study from first principles these effects in single-layer and bilayer graphene doped with various alkali and alkaline earth metals. I find new dopantactivated damping channels: loss due to out-of-plane graphene and in-plane dopant vibrations, and electron transitions between graphene and dopant states. The latter excitations interact with the graphene plasmon and together they form a new hybrid mode. The study points out a strong dependence of these features on the type of dopants and the number of layers, which could be used as a tuning mechanism in future graphene-based plasmonic devices. Recently, the quantized collective motion of surface electrons, called surface plasmon, has gained renewed attention as the potential mechanism for the confinement of electromagnetic energy, which could reduce the size of optical devices to the desired nanoscale.1 The twodimensional (2D) plasmon of graphene is a most promising framework to investigate these confinement effects, 2 as a result of its relatively long lifetime 3-5 and its tunability through an electrostatic gating 6,7 or chemical doping. [8][9][10] Angle-resolved photoemission (ARPES) studies show that chemical doping by deposition of alkali and alkaline earth metal (X) atoms on graphene introduces much higher concentrations of conducting electrons than the standard electrostatic gating techniques. 8,11,12 In fact, two recent theoretical studies point out that lithium-doped single-and few-layer graphene can support plasmons ranging from nearinfrared to possibly visible energies due to a high level of doping. 9,10 This opens new possibilities to extend the application of graphene plasmonics to telecommunication technologies,photodetectors, 13 or photovoltaic systems.
14The underlying physics of dopant-induced plasmon decay in graphene, i.e., how dopants affect the electron scattering processes, is not understood yet. The largest contribution consists of interband electron-hole pair excitations between occupied and unoccupied π bands 3 (i.e., Landau damping), which are suppressed due to Pauli blocking below the value of two times the Fermi energy, 2ε F . Since the value of ε F in X-doped graphene shifts up to ∼ 1.5 eV, 8,11,12 this damping channel is diminished within a large energy window. Nevertheless, the 2D plasmon in doped graphene can still show substantial decay rates below the interband gap because of higher-order processes: electron-phonon, 3,4,15,16 electron-impurity,
17and electron-electron 18,19 scatterings. For the case of dopant-free graphene it is widely accepted that the first decay channel is a major contributor to the plasmon decay rate, but only when the plasmon energy exceeds the energy of intrinsic optical phonon of graphene (ω op ≈ 0.2 eV). 3,4 On the other hand, when the plasmon ene...