Temperature Dependence of Phonon Energies and Lifetimes in Single-and Few-layered Graphene

In this work, we have studied the phonon properties of multi-layered graphene with the use of Molecular Dynamics (MD) simulations and the k-space Autocorrelation Sequence (k-VACS) method. We calculate the phonon dispersion curves, densities of states and lifetimes τ of few-layered graphene of 1-5 layers and graphite. Γ-point phonon energies and lifetimes are investigated for different temperatures ranging from 80 K to 1000 K. The study focuses on the impact of the interlayer interaction and temperature on the energies and lifetimes of the Γ-point phonons, as well as the type of interlayer potential used. For the later we used the Kolmogorov-Crespi (KC) and the Lennard-Jones (LJ) potentials. We have found that the number of layers N has little effect on the intra-layer (ZO and G) mode energies and greater effect on the inter-layer (Layer Shearing and Layer Breathing) modes, while τ is generally affected by N for all modes, except for the Layer Shear mode. The trend of N on the lifetimes was also found to independent of the type of potential used. For the Raman-active G phonon, our calculations show that the lifetime increase with N and that this increase is directly connected to the strength of the interlayer coupling and how this is modelled.