Influence of point defects and multiscale pores on the different phonon transport regimes

A common strategy to tailor the thermal conductivity of a material is to introduce structural features that modulate phonon scattering, such as atomic-scale defects and nano- and macro-sized pores. However, particle-like and wave-like phonon transport and scattering during a crossover in thermal transport regimes is not well understood. Here, we perform a rigorous quantitative comparison of the thermal conductivity obtained from molecular dynamics simulations and phonon Boltzmann transport equations, taking graphene as an example. We observe a generally increasing trend in thermal conductivity when the pore size increases from point defect to nanopore, due to a transition from Rayleigh scattering to geometric scattering and reduced boundary density. The thermal conductivity further converges to the diffusive limit for macropores because of the dominant effect of phonon-phonon scattering over phonon-boundary scattering. Moreover, we identify a critical interpore distance for the crossover from dependent to independent phonon-pore scattering and a critical pore size for the crossover from point defect scattering to boundary scattering. This work provides a comprehensive understanding of phonon transport in materials containing defects and pores.