Phonon thermal transport in strained and unstrained graphene from first principles

TLDR

The study investigates phonon thermal transport in graphene using first‑principles techniques to elucidate its mechanisms. The authors use a first‑principles Boltzmann‑Peierls equation to calculate the lattice thermal conductivity of strained and unstrained graphene. The calculations reveal that flexural acoustic phonons dominate graphene’s lattice thermal conductivity, which is largely strain‑insensitive, agrees with experiment, and shows only modest improvement from isotopic purification due to strong anharmonic scattering.

Abstract

A rigorous first principles Boltzmann-Peierls equation (BPE) for phonon transport approach is employed to examine the lattice thermal conductivity, ${\ensuremath{\kappa}}_{L}$, of strained and unstrained graphene. First principles calculations show that the out-of-plane, flexural acoustic phonons provide the dominant contribution to ${\ensuremath{\kappa}}_{L}$ of graphene for all strains, temperatures, and system sizes considered, supporting a previous prediction that used an optimized Tersoff empirical interatomic potential. For the range of finite system sizes considered, we show that the ${\ensuremath{\kappa}}_{L}$ of graphene is relatively insensitive to strain. This provides validation for use of the BPE approach to calculate ${\ensuremath{\kappa}}_{L}$ for unstrained graphene, which has recently been called into question. The temperature and system size dependence of the calculated ${\ensuremath{\kappa}}_{L}$ of graphene is in good agreement with experimental data. The enhancement of ${\ensuremath{\kappa}}_{L}$ with isotopic purification is found to be relatively small due to strong anharmonic phonon-phonon scattering. This work provides insight into the nature of phonon thermal transport in graphene, and it demonstrates the power of first principles thermal transport techniques.