Thermo-Mechanical Characterization and Interfacial Thermal Resistance Studies of Chemically Modified Carbon Nanotube Thermal Interface Material - Experimental and Mechanistic Approaches

Abstract

Effective application of thermal interface materials (TIM) sandwiched between silicon and a heat spreader in a microelectronic package for improved heat dissipation is studied through thermal and mechanical characterization of high thermally conductive carbon nanotubes (CNTs) integrated into eutectic gallium indium liquid metal (LM) wetting matrix. Thermal conductivity data from Infrared microscopy tool reveals the dependence of experimental factors such as matrix types, TIM contacting interfaces, orientation of CNTs and wetting of CNTs in the matrix on the thermal behavior of TIM composite. Observed generalized trend on LM-CNT TIM shows progressive decrease in effective thermal conductivity with increasing CNT volume fractions. Further thermal characterizations LM-CNT TIM however show over 2x increase in effective thermal conductivity over conventional polymer TIMs (i.e. TIM from silicone oil matrix) but fails to meet 10x improvement expected. Poor wetting of CNT with LM matrix is hypothesized to hinder thermal improvement of LM-CNT TIM composite. Thus, wetting enhancement technique through electro-wetting and liquid crystal (LC) based matrix proposed to enhance CNT-CNT contact in LM-CNT TIM results in thermal conductivity improvement of 40 to 50% with introduction of voltage gradient of 2 to 24 volts on LM-CNT TIM sample with 0.1 to 1 percent CNT volume fractions over non voltage LM-CNT TIM test samples. Key findings through this study show that voltage tests on LC- CNT TIM can cause increased CNT-CNT networks resulting in 5x increase in thermal conductivity over non voltage LC-CNT TIM and over 2x improvement over silicone-CNT TIMs. Validation of LM wetting of CNT hypothesis further shows that wetting and interface adhesion mechanisms are not the only factors required to improve thermal performance of LM-CNT TIM. Anisotropic characteristic of thermal conductivity of randomly dispersed CNTs is a major factor causing lower thermal performance of LM-CNTs TIM composite. Other factors resulting in LM-CNT TIM decreasing thermal conductivity with increasing CNT loading are (i) Lack of CNT-CNT network due to large difference in surface tension and mass density between CNTs and LM in TIM composite (ii) Structural stability of MWCNT and small MFP of phonons in ~5um MWCNTs compared to the system resulted in phonon scattering with reduced heat flow (iii) CNT percolation threshold limit not reached owing to thermal shielding due to CNT tube interfacial thermal resistance. While mixture analytical models employed are able to predict thermal behaviors consistent with CNT-CNT network and CNT- polymer matrix contact phenomenon, these models are not equipped to predict thermo-chemical attributes of CNTs in LM-CNT TIM. Extent of LM-CNT wetting and LM-solid surface interfacial contact impacts on interfacial thermal resistance are investigated through LM contact angle, XPS/AES and SEM-EDX analyses on Au/Ni and Ni coated copper surfaces. Contact angle measurements in the range of 120o at both 55oC and 125oC show non wetting of LM on CNT, Au and Ni surfaces. Interface reactive wetting elemental composition of 21 days aged LM on Au/Ni and Ni surfaces reveals Ga dissolution in Au and Ni diffusion of ~0.32um in Au which are not present for similar analysis of 1 day LM on Au/Ni surface. Formation of Au-Ni-Ga IMC and IMC-oxide iono-covalency occurrence at the interface causes reduction in surface tension and reduction in interfacial contact resistance.