Exploring Trade-offs in Thermal Interface Materials: The Impact of Polymer-Filler Interfaces on Thermal Conductivity and Thixotropy

Effective thermal transport across solid-solid interfaces, essential in thermal interface materials (TIMs), necessitates both optimal thixotropy and high thermal conductivity. The role of filler surface modification, a fundamental aspect of TIM fabrication, in influencing these properties is not fully understood. This study employs the use of a silane coupling agent (SCA) to modify alumina, integrating experimental approaches with molecular dynamics simulations, to elucidate the interface effects on thixotropy and thermal conductivity in polydimethylsiloxane (PDMS)-based TIMs. Our findings reveal that varying SCAs modify both interface binding energy and transition layer thickness. The interface binding energy restricts macromolecular segmental relaxation near the interface, hindering desirable thixotropy and bond line thickness. Conversely, the transition layer thickness at the interface positively influences thermal conductivity, facilitating phonon transport between the polymer and filler. Consequently, selecting an optimal SCA enables a balance between traditionally conflicting goals of high thermal conductivity and minimal bond line thickness, achieving an impressively low interface thermal resistance of just 2.45–4.29 K·mm²·W⁻¹ at 40 psi.