The critical particle size for enhancing thermal conductivity in metal nanoparticle-polymer composites

Polymers used as thermal interface materials are often filled with high-thermal conductivity particles to enhance the thermal performance. Here, we have combined molecular dynamics and the two-temperature model in 1D to investigate the impact of the metal filler size on the overall thermal conductivity. A critical particle size has been identified above which thermal conductivity enhancement can be achieved, caused by the interplay between high particle thermal conductivity and the added electron-phonon and phonon-phonon thermal boundary resistance brought by the particle fillers. Calculations on the SAM/Au/SAM (self-assembly-monolayer) system show a critical thickness Lc of around 10.8 nm. Based on the results, we define an effective thermal conductivity and propose a new thermal circuit analysis approach for the sandwiched metal layer that can intuitively explain simulation and experimental data. The results show that when the metal layer thickness decreases to be much smaller than the electron-phonon cooling length (or as the “thin limit”), the effective thermal conductivity is just the phonon portion, and electrons do not participate in thermal transport. As the thickness increases to the “thick limit,” the effective thermal conductivity recovers the metal bulk value. Several factors that could affect Lc are discussed, and it is discovered that the thermal conductivity, thermal boundary resistance, and the electron-phonon coupling factor are all important in controlling Lc.