Gecko-inspired adhesive structures enable efficiently thermal conductance and vibration dissipation in a highly mismatched system

There is often a trade-off between thermal conductance and vibration dissipation of polymer-based thermal interface materials (TIMs). Achieving efficient thermal management requires a sufficiently high filler content, however, which in turn raises the storage modulus of TIMs and thus compromises their damping performances. Inspired by Nature's climbers of geckos, we envisage that the abundant short dangling ends of the comb-brush copolymers, like the gecko feet-hairs structures, could comfort to the highly mismatched interfaces between constituent materials (TIMs/substrate) and inside composites (polymer/fillers). Control experiments reveal that the short molecular hair structures are typically positively correlated with thermal boundary conductance of polymer-based TIM composites, which is contrary to the usual understanding in pure polydimethylsiloxane systems. Tailoring the weight ratio of comb-brush copolymers offers the optimal thermal conductivity (4.9 +/- 0.1 W.K-- 1.(- 1)) and contact thermal resistance (0.2 +/- 0.05 K.cm(2.)W(-1)). Additionally, the dissociation of van der Waals interaction between polymer/fillers and the broadened relaxation spectrum efficiently dissipate the vibration energy, endowing TIMs with excellent damping capacity over a broad frequency range (> 0.5 Hz). This study points out a promising direction for next-generation high-performance TIMs, powering the development of intelligent connected vehicles.