Bimodal grain-size scaling of thermal transport in polycrystalline graphene from large-scale molecular dynamics simulations

TL;DR

This study uses large-scale molecular dynamics simulations to reveal bimodal grain-size scaling of thermal conductivity in polycrystalline graphene, emphasizing the dominant role of out-of-plane phonons and the necessity of quantum corrections for experimental agreement.

Contribution

It introduces a bimodal scaling model with two effective Kapitza lengths for thermal transport in polycrystalline graphene, highlighting the importance of out-of-plane phonons.

Findings

Thermal conductivity scales bimodally with grain size.

Out-of-plane phonons dominate the thermal transport.

Quantum corrections are essential for matching experimental data.

Abstract

Grain boundaries in graphene are inherent in wafer-scale samples prepared by chemical vapor deposition. They can strongly influence the mechanical properties and electronic and heat transport in graphene. In this work, we employ extensive molecular dynamics simulations to study thermal transport in large suspended polycrystalline graphene samples. Samples of different controlled grain sizes are prepared by a recently developed efficient multiscale approach based on the phase field crystal model. In contrast to previous works, our results show that the scaling of the thermal conductivity with the grain size implies bimodal behaviour with two effective Kapitza lengths. The scaling is dominated by the out-of-plane (flexural) phonons with a Kapitza length that is an order of magnitude larger than that of the in-plane phonons. We also show that in order to get quantitative agreement with the most recent experiments, quantum corrections need to be applied to both the Kapitza conductance of grain boundaries and the thermal conductivity of pristine graphene and the corresponding Kapitza lengths must be renormalized accordingly.