Soft polymer composites with improved thermal conductivity are needed for the thermal management of electronics. Interfacial thermal boundary resistance, however, prevents the efficient use of many high thermal conductivity fill materials. Magnetic alignment of ferrous fill material enforces percolation of the high thermal conductivity fill, thereby shifting the governing boundary resistance to the particle- particle interfaces and increasing the directional thermal conductivity of the polymer composite. Magnetic alignment maximizes the thermal conductivity while minimizing composite stiffening at a fill fraction of half the maximum packing factor. The directional thermal conductivity of the composite is improved by more than 2-fold. Particle-particle contact engineering is then introduced to decrease the particle- particle boundary resistance and further improve the thermal conductivity of the composite.

The interface between rigid fill particles is a point contact with very little interfacial area connecting them. Silver and gallium-based liquid metal (LM) coatings provide soft interfaces that, under pressure, increase the interfacial area between particles and decrease the particle-particle boundary resistance. These engineered contacts are investigated both in and out of the polymer matrix and with and without magnetic alignment of the fill. Magnetically aligned in the polymer matrix, 350nm- thick silver coatings on nickel particles produce a 1.8-fold increase in composite thermal conductivity over the aligned bare-nickel composites. The LM coatings provide similar enhancements, but require higher volumes of LM to do so. This is due to the rapid formation of gallium oxide, which introduces additional thermal boundaries and decreases the benefit of the LM coatings.

The oxide shell of LM droplets (LMDs) can be ruptured using pressure. The pressure needed to rupture LMDs matches closely to thin-walled pressure vessel theory. Furthermore, the addition of tungsten particles stabilizes the mixture for use at higher pressures. Finally, thiols and hydrochloric acid weaken the oxide shell and boost the thermal performance of the beds of LMDs by 50% at pressures much lower than 1 megapascal (MPa) to make them more suitable for use in TIMs.