Phonons in potassium-doped graphene: The effects of electron-phonon interactions, dimensionality, and adatom ordering

Graphene phonons are measured as a function of electron doping via the addition of potassium adatoms. In the low doping regime, the in-plane carbon G peak hardens and narrows with increasing doping, analogous to the trend seen in graphene doped via the field effect. At high dopings, beyond those accessible by the field effect, the G peak strongly softens and broadens. This is interpreted as a dynamic, nonadiabatic renormalization of the phonon self-energy. At dopings between the light and heavily doped regimes, we find a robust inhomogeneous phase where the potassium coverage is segregated into regions of high and low density. The phonon energies, linewidths, and tunability are notably very similar for one- to four-layer potassium-doped graphene, but significantly different to bulk potassium-doped graphite.