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Uniaxiality-Induced Reduced-Pressure Synthesis of Ultrahard Paracrystalline Diamond

Yue Pan,Xiaohong Yuan,Yong Cheng,Baoyin Xu,Shucheng Liu,Zhitong Wang,Shida Wang,Kuo Hu,Shengcai Zhu,Quanjun Li,Ming-sheng Wang,Zhaodong Liu,Hu Tang,Bingbing Liu

Synthesizing fully sp 3 -bonded non-crystalline carbon remains a long-standing challenge due to the intrinsic instability of the sp 3 bond at ambient pressure. Recently, paracrystalline diamond, a new-form sp 3 -bonded non-crystalline carbon consisting of sub-nanometer-sized paracrystallites, has been synthesized from face-centered cubic C 60 at 30 GPa, which has attracted attention due to its unique structural features and excellent physical properties. However, the ultrahigh synthesis pressure of paracrystalline diamond poses an obstacle to its large-scale production and applications. In this study, paracrystalline diamond is synthesized at an exceptionally low pressure (16 GPa) via inducing uniaxiality at high-pressure and high-temperature conditions, thereby breaking through the temperature-pressure phase diagram of C 60 . By combining structural characteristics and advanced molecular dynamics simulation, the remarkable reduction of synthesis pressure is attributed to the fact that the symmetry of the C 60 cage is broken due to the uniaxiality, which further allows the C 60 cage to collapse at much lower pressures. This work reveals the critical role of uniaxiality in the reduced-pressure synthesis of paracrystalline diamond, which may provide a potent methodological strategy for the development of novel low-cost high-pressure materials.