Quantum-corrected thickness-dependent thermal conductivity in amorphous silicon predicted by machine-learning molecular dynamics simulations

Abstract: Amorphous silicon (a-Si) is an important thermal-management material and also serves as an ideal playground for studying heat transport in strongly disordered materials. Theoretical prediction of the thermal conductivity of a-Si in a wide range of temperatures and sample sizes is still a challenge. Herein we present a systematic investigation of the thermal transport properties of a-Si by employing large-scale molecular dynamics (MD) simulations with an accurate and efficient machine-learned neuroevolution potential (NEP) trained against abundant reference data calculated at the quantum-mechanical density-functional-theory level. The high efficiency of NEP allows us to study the effects of finite size and quenching rate in the formation of a-Si in great detail. We find that it requires a simulation cell up to $64,000$ atoms (a cubic cell with a linear size of 11 nm) and a quenching rate down to $10^{11}$ K s$^{-1}$ for fully convergent thermal conductivity. Structural properties, including short- and medium-range order as characterized by the pair correlation function, angular distribution function, coordination number, ring statistics and structure factor are studied to demonstrate the accuracy of NEP and to further evaluate the role of quenching rate. Using both the heterogeneous and the homogeneous nonequilibrium MD methods and the related spectral decomposition techniques, we calculate the temperature- and thickness-dependent thermal conductivity values of a-Si and show that they agree well with available experimental results from 10 K to room temperature. Our results also highlight the importance of quantum effects in the calculated thermal conductivity and support the quantum correction method based on the spectral thermal conductivity.