Symmetry-dependent dielectric screening of optical phonons in monolayer graphene

Abstract

Quantised lattice vibrations (i.e., phonons) in solids are robust and unambiguous fingerprints of crystal structures and of their symmetry properties. In metals and semimetals, strong electron-phonon coupling may lead to so-called Kohn anomalies in the phonon dispersion, providing an image of the Fermi surface in a non-electronic observable. Kohn anomalies become prominent in low-dimensional systems, in particular in graphene, where they appear as sharp kinks in the in-plane optical phonon branches. However, in spite of intense research efforts on electron-phonon coupling in graphene and related van der Waals heterostructures, little is known regarding the links between the symmetry properties of optical phonons at and near Kohn anomalies and their sensitivity towards the local environment. Here, using inelastic light scattering (Raman) spectroscopy, we investigate a set of custom-designed graphene-based van der Waals heterostructures, wherein dielectric screening is finely controlled at the atomic layer level. We demonstrate experimentally and explain theoretically that, depending exclusively on their symmetry properties, the two main Raman modes of graphene react differently to the surrounding environment. While the Raman-active near-zone-edge optical phonons in graphene undergo changes in their frequencies due to the neighboring dielectric environment, the in-plane, zone-centre optical phonons are symmetry-protected from the influence of the latter. These results shed new light on the unique electron-phonon coupling properties in graphene and related systems and provide invaluable guidelines to characterise dielectric screening in van der Waals heterostructures and moir\'e superlattices.