Soft thermal interface materials (TIMs) are critical for improving the thermal management of advanced microelectronic devices. Despite containing high thermal conductivity filler materials, TIM performance is limited by thermal resistances between fillers, filler-matrix, and external contact resistance. Recently, room-temperature liquid metals (LMs) started to be adapted as an alternative TIM for their low thermal resistance and fluidic nature. However, LM-based TIMs face challenges due to their low viscosity, non-wetting qualities, chemical reactivity, and corrosiveness towards aluminum.To address these concerns, this dissertation research investigates fundamental LM properties and assesses their utility for developing multiphase LM composites with strong thermal properties. Augmentation of LM with gallium oxide and air capsules lead to LM-base foams with improved spreading and patterning. Gallium oxides are responsible for stabilizing LM foam structures which is observed through electron microscopy, revealing a temporal evolution of air voids after shear mixing in air. The presence of air bubbles and oxide fragments in LM decreases thermal conductivity while increasing its viscosity as the shear mixing time is prolonged. An overall mechanism for foam generation in LM is presented in two stages: 1) oxide fragment accumulation and 2) air bubble entrapment and propagation. To avoid the low thermal conductivity air content, mixing of non-reactive particles of tungsten or silicon carbide (SiC) into LM forms paste-like LM-based mixtures that exhibit tunable high thermal conductivity 2-3 times beyond the matrix material. These filler materials remain chemically stable and do not react with LM over time while suspended. Gallium oxide-mediated wetting mechanisms for these non-wetting fillers are elucidated in oxygen rich and deficient environments. Three-phase composites consisting of LM and Ag-coated SiC fillers dispersed in a noncuring silicone oil matrix address LM-corrosion related issues. Ag-coated SiC particles enable improved wetting of the LM, and the results show that applied pressure is necessary for bridging of these LM-coated particles to improve filler thermal resistance. Compositional tuning between the fillers leads to thermal improvements in this multiphase composite. The results of this dissertation work aim to advance our current understanding of LMs and how to design LM-based composite materials for improved TIMs and other soft thermal applications.

A new class of layered materials called the transition metal trichalcogenides (TMTCs) exhibit strong anisotropic properties due to their quasi-1D nature. These 2D materials are composed of chain-like structures which are weakly bound to form planar sheets with highly directional properties. The vibrational properties of three materials from the TMTC family, specifically TiS3, ZrS3, and HfS3, are relatively unknown and studies performed in this work elucidates the origin of their Raman characteristics. The crystals were synthesized through chemical vapor transport prior to mechanical exfoliation onto Si/SiO¬2 substrates. XRD, AFM, and Raman spectroscopy were used to determine the crystallinity, thickness, and chemical signature of the exfoliated crystals. Vibrational modes and anisotropic polarization are investigated through density functional theory calculations and angle-resolved Raman spectroscopy. Particular Raman modes are explored in order to correlate select peaks to the b-axis crystalline direction. Mode III vibrations for TiS3, ZrS3, and HfS3 are shared between each material and serves as a unique identifier of the crystalline orientation in MX3 materials. Similar angle-resolved Raman studies were conducted on the novel Nb0.5Ti0.5S3 alloy material grown through chemical vapor transport. Results show that the anisotropy direction is more difficult to determine due to the randomization of quasi-1D chains caused by defects that are common in 2D alloys. This work provides a fundamental understanding of the vibrational properties of various TMTC materials which is needed to realize applications in direction dependent polarization and linear dichroism.