Low Dielectric Constant and Low Thermal Expansion Coefficient Polyimide with Oxazole Ring Structure in the Main Chain
摘要
With the rapid development of microelectronic devices towards higher frequency, high speed, miniaturization, and high integration, there is a growing need for interlayer dielectric materials with a low dielectric constant (ε) and coefficient of thermal expansion (CTE). Traditional aromatic polyimides with ε ranging from 3.2 to 3.6 and CTEs exceeding 60 ppm/K cannot meet the requirements of modern 5G communications, integrated circuits, and advanced packaging. In this paper, a hydroxyl-containing polyimide was synthesized by thermal polycondensation of 2,2-bis(4-hydroxy-3-aminophenyl) propane (BAP), 4,4′-diaminodiphenyl ether (ODA) and 1,2,4,5-benzotetraacetic anhydride (PMDA) with aminopropyl heptyl-terminated poly(dicyclohexylsiloxane) (NH2-POSS) as the end-capping agent. Subsequently, thermal rearrangement reactions between hydroxyl groups and imine rings at high temperatures were conducted to prepare a polyimide with low ε and CTE and an oxazole ring structure in the main chain (Re-xBAP-PI). The thermal rearrangement reactions reduced the CTE value of Re-xBAP-PI to 19.6–25.4 ppm/K, and the introduction of NH2-POSS effectively lowered the dielectric constant of the Re-xBAP-PI samples. The Re-2BAP-PI samples demonstrated a dielectric constant of 2.79 at 200 kHz, a CTE of 26.3 ppm/K, a breakdown strength of 177.41 kV/mm, and a water absorption rate of 2.47%. Given these exceptional properties, the polyimide materials synthesized through this method are expected to provide novel interlayer dielectric materials with low ε and CTE.