Non-negligible Contributions to Thermal Conductivity From Localized Modes in Amorphous Silicon Dioxide.

Thermal conductivity is important for almost all applications involving heat transfer. The theory and modeling of crystalline materials is in some sense a solved problem, where one can now calculate their thermal conductivity from first principles using expressions based on the phonon gas model (PGM). However, modeling of amorphous materials still has many open questions, because the PGM itself becomes questionable when one cannot rigorously define the phonon velocities. In this report, we used our recently developed Green-Kubo modal analysis (GKMA) method to study amorphous silicon dioxide (a-SiO). The predicted thermal conductivities exhibit excellent agreement with experiments and anharmonic effects are included in the thermal conductivity calculation for all the modes in a-SiO for the first time. Previously, localized modes (locons) have been thought to have a negligible contribution to thermal conductivity, due to their highly localized nature. However, in a-SiO our results indicate that locons contribute more than 10% to the total thermal conductivity from 400 K to 800 K and they are largely responsible for the increase in thermal conductivity of a-SiO above room temperature. This is an effect that cannot be explained by previous methods and therefore offers new insight into the nature of phonon transport in amorphous/glassy materials.