Towards high-performance polydimethylsiloxane-based materials for thermal management: A molecular dynamics study

To efficiently design high-performance polymer-based thermal interface material (TIM), it is imperative to investigate how microstructural influences thermal transport. Utilizing molecular dynamics (MD) simulations, this study examined the effects of crosslinking degree (10–40%) and alumina (Al2O3) filler doping ratios (0–23.13 wt%) on the thermomechanical behaviors of PDMS. Our findings indicated that increasing the degree of crosslinking significantly enhances thermal conductivity at lower doping rates by creating additional heat transfer channels. However, at higher doping rates, thermal conductivity improvement is mitigated due to the potential hindrance caused by fillers. Optimal thermal conductivity was observed with a 20% crosslinking degree and 14.67 wt% Al2O3 doping, achieving an 18% enhancement compared to systems without crosslinking. These results underscore the complex interplay between crosslinking and filler content in optimizing the thermal performance of PDMS-based TIMs, contributing to the advancement of materials for efficient thermal management in microelectronic devices.