“…Now, considerable attention has been paid to the development of high- k materials, and many attempts at highly thermally conductive TIMs have been witnessed in the past two decades. − For example, carbon nanotubes (CNTs) are the ideal TIM precursor due to their one-dimensionally highly thermo-conductive characteristic (≥2000 W/m K) . Various vertically aligned technologies were adopted to successfully fabricate perpendicular CNTs-array TIMs, whose out-of-plane k were reported to be able to exceed 70 W/m K. , Similar results can also be found in vertical graphene TIMs, for example, a mechanical-machining processed graphene monolith was manifested to exhibit an out-of-plane k as high as 143 W/m K, which is on par with some metals and alloys. , In addition to the above high- k carbons, other TIMs include liquid metals, ,, inherently thermally conductive polymers, polymer composites (i.e., thermal grease, gel, and pad), − and phase change materials. − Looking at the previously reported TIMs, the manipulation of the anisotropic k and making it superb in the thickness direction is not a very difficult thing; however, the achievement of a low R eff when these TIMs are applied in a sandwiched heat source-sink structure remains a formidable challenge. Taking one of the most mature and commercial dry-contact TIMs (thermal grease) as an example, its applied thermal resistance in a sandwiched structure is rarely found to be lower than 5 mm 2 K/W, a boundary value that traditional solders can perform .…”