Strong magnetophonon resonance induced triple G-mode splitting in graphene on graphite probed by micromagneto Raman spectroscopy

The resonance between the G-band phonon excitation and Landau level optical transitions in graphene has been systematically studied by micromagneto Raman mapping. In purely decoupled graphene regions on a graphite substrate, eight traces of anticrossing spectral features with G-mode peaks are observed as a function of magnetic fields up to 9 T, and these traces correspond to either symmetric or asymmetric Landau level transitions. Three distinct split peaks of the G mode, named G_-, G_i, and G₊, are observed at the strong magnetophonon resonance condition corresponding to a magnetic field of ∼4.65 T. These three special modes are attributed to (i) the coupling between the G phonon and the magneto-optical transitions, which is responsible for G₊ and G_- and can be well described by the two coupled mode model and (ii) the magnetic field-dependent oscillation of the G_i band, which is currently explained by the G band of graphite modified by the interaction with G₊ and G_-. The pronounced interaction between Dirac fermions and phonons demonstrates a dramatically small Landau level width (∼1.3 meV), which is a signature of the ultrahigh quality graphene obtained on the surface of graphite.