Acoustic Phonon Lifetimes and Thermal Transport in Free-Standing and Strained Graphene

We use first-principles methods based on density functional perturbation theory to characterize the lifetimes of the acoustic phonon modes and their consequences on the thermal transport properties of graphene. We show that using a standard perturbative approach, the transverse and longitudinal acoustic phonons in free-standing graphene display finite lifetimes in the long-wavelength limit, making them ill-defined as elementary excitations in samples of dimensions larger than ∼1 μm. This behavior is entirely due to the presence of the quadratic dispersions for the out-of-plane phonon (ZA) flexural modes that appear in free-standing low-dimensional systems. Mechanical strain lifts this anomaly, and all phonons remain well-defined at any wavelength. Thermal transport is dominated by ZA modes, and the thermal conductivity is predicted to diverge with system size for any amount of strain. These findings highlight strain and sample size as key parameters in characterizing or engineering heat transport in graphene.