High-density electronics are hindered by the constraints of Sn-based solder joints, necessitating the exploration of Cu–Cu solid-state bonding. However, current bonding methods are expensive and time-consuming; therefore, understanding the Cu–Cu bonding mechanism is crucial for optimization. This study utilizes molecular dynamics (MD) simulation to elucidate the Cu–Cu solid-state bonding behavior, focusing on interfacial densification and diffusion phenomena. Furthermore, it highlights the influence of crystal orientation on the interfacial bonding behavior. To analyze the impact of crystal orientation, monocrystalline Cu slabs with a simplified periodic surface structure were employed to replicate surface roughness and subsequently bonded at a specific temperature. The results indicate the critical influence of crystalline orientations on the bonding process: identical orientations result in slower densification at the interface, whereas misoriented orientations significantly accelerate it. This effect, attributed to the grain boundary (GB) structures formed owing to misorientation, suggests a central role for GB diffusion in bonding progression. Diffusion coefficients calculated using the mean square displacement (MSD) confirmed these findings and exhibited significantly larger values for misoriented joints. Additionally, the simulations reveal an activation energy for GB diffusion that is lower than conventional values, highlighting the impact of the crystallographic orientation and voids at the bonding interface. Our research elucidates the role of crystalline orientation in diffusion phenomena at bonding interfaces, offering valuable implications for optimizing bonding-based manufacturing processes.

The evolution of the transient liquid-phase sintered (TLPS) Cu–Sn skeleton microstructure during thermal aging was evaluated to clarify the thermal reliability for die-attach applications. The Cu–Sn skeleton microstructure, which consists of Cu particles connected with Cu–Sn intermetallic compounds partially filled with polyimide resin, was obtained by the pressure-less TLP sintering process at 250 °C for 1 min using a novel Cu-solder-resin composite as a bonding material in a nitrogen atmosphere. Experimental results indicate that the TLPS joints were mainly composed of Cu, Cu₆Sn₅, and Cu₃Sn in the as-bonded state, where submicron voids were observed at the interface between Cu₃Sn and Cu particles. After thermal aging at 150, 175, and 200 °C for 1000 h, the Cu₆Sn₅ phase fully transformed into Cu₃Sn except at the chip-side interface, where the number of the submicron voids appeared to increase. The averaged shear strengths were found to be 22.1 (reference), 22.8 (+3%), 24.0 (+9%), and 19.0 MPa (−14%) for the as-bonded state and specimens aged at 150, 175, and 200 °C for 1000 h, respectively. The TLPS joints maintained a shear strength over 19 MPa after thermal aging at 200 °C for 1000 h because of both the positive and negative impacts of the thermal aging, which include the transformation of Cu₆Sn₅ into Cu₃Sn and the formation of submicron voids at the interface, respectively. These results indicate an excellent thermal reliability of the TLPS Cu–Sn skeleton microstructure.