A review on advanced carbon-based thermal interface materials for electronic devices

Modern microelectronics and emerging technologies such as wearable devices and soft robotics require conformable and thermally conductive thermal interface materials to improve their performance and longevity. Gallium-based liquid metals (LMs) are promising candidates for these applications yet are limited by their moderate thermal conductivity, difficulty in surface-spreading, and pump-out issues. Incorporation of metallic particles into the LM can address these problems, but observed alloying processes shift the LM melting point and lead to undesirable formation of additional surface roughness. Here, these problems are addressed by introducing a mixture of tungsten microparticles dispersed within a LM matrix (LM-W) that exhibits two- to threefold enhanced thermal conductivity (62 ± 2.28 W m-1 K-1 for gallium and 57 ± 2.08 W m-1 K-1 for EGaInSn at a 40% filler volume mixing ratio) and liquid-to-paste transition for better surface application. It is shown that the formation of a nanometer-scale LM oxide in oxygen-rich environments allows highly nonwetting tungsten particles to mix into LMs. Using in situ imaging and particle dipping experimentation within a focused ion beam and scanning electron microscopy system, the oxide-assisted mechanism behind this wetting process is revealed. Furthermore, since tungsten does not undergo room-temperature alloying with gallium, it is shown that LM-W remains a chemically stable mixture.

Oxide-Mediated Formation of Chemically Stable Tungsten-Liquid Metal Mixtures for Enhanced Thermal Interfaces.

A review of carbon-based thermal interface materials: mechanism, thermal measurements and thermal properties

Gallium-based liquid metal (LM) composite with metallic fillers is an emerging class of thermal interface materials (TIMs), which are widely applied in electronics and power systems to improve their performance. In situ alloying between gallium and many metallic fillers like copper and silver, however, leads to a deteriorated composite stability. This paper presents an interfacial engineering approach using 3-chloropropyltriethoxysilane (CPTES) to serve as effective thermal linkers and diffusion barriers at the copper-gallium oxide interfaces in the LM matrix, achieving an enhancement in both thermal conductivity and stability of the composite. By mixing LM with copper particles modified by CPTES, a thermal conductivity (κ) as high as 65.9 W m-1 K-1 is achieved. In addition, κ can be tuned by altering the terminal groups of silane molecules, demonstrating the flexibility of this approach. The potential use of such composite as a TIM is also shown in the heat dissipation of a computer central processing unit. While most studies on LM-based composites enhance the material performance via direct mixing of various fillers, this work provides a different approach to fabricate high-performance LM-based composites and may further advance their applications in various areas including thermal management systems, flexible electronics, consumer electronics, and biomedical systems.

Liquid Metal Composites with Enhanced Thermal Conductivity and Stability Using Molecular Thermal Linker.

Critical Review on the Physical Properties of Gallium-Based Liquid Metals and Selected Pathways for Their Alteration

The focus of this paper is how to efficiently enhance the thermal conductance of gallium-based thermal interface materials (TIMs) and greatly avoid the excessive consumption of liquid metal during its application. Highly heat-conducting diamond particles are selected as the reinforced additives for pure gallium on account of their mature technology of surface metallization. To improve the interface combination status between those inorganic fillers and liquid metal matrix, chromium transition layer is deposited on the surfaces of diamond particles by magnetron sputtering method. The phase composition of cladding layer on diamond particles is analyzed by transmission electron microscopy combined with focused ion beam technology. To measure the thermal conductivity of gallium-based TIM filled with chromium-coated diamond particles, a specific three-layer structure sample is made for laser flash analysis and the corresponding theoretical fitting model is deduced subsequently. After performing iterative solution through programming, our results present that 47 wt% addition of chromium-coated diamond particles can dramatically increase the thermal conductivity of pure gallium from 29.3 to 112.5 W/(m·K) at room temperature. And fortunately, it has not yet been observed that the chromium coating is over consumed by liquid metal or the thermal conductivity of composite seriously degrades after thermal aging treatment at 80 °C for 192 h, strongly indicating that chromium could be used as the diffusion barrier layer for heat-conducting particles and the metal substrates to maintain long-term reliable service of gallium-based TIMs.

Investigation on enhancing the thermal conductance of gallium-based thermal interface materials using chromium-coated diamond particles

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Investigation on enhancing the thermal conductance of gallium-based thermal interface materials using chromium-coated diamond particles