Contemporary lifestyle is interwoven with technological achievements that implement the use of permanent magnets. Polynuclear lanthanide single-molecule magnets (SMMs) lack strong magnetic communication, which renders the design of high-performing SMMs an ongoing challenge. To overcome this, incorporation of radical pyrazine (pyz^⋅−) linkers between lanthanides is a compelling approach. Careful tuning of the synthetic conditions led to dinuclear [(Cp∗₂Ln^III)₂(pyz^⋅−)(THF)₂][BPh₄] (Ln = Gd (1), Dy (2); Cp∗ = pentamethylcyclopentadienyl; THF = tetrahydrofuran) and tetranuclear [(Cp∗₂Ln^III)₄(pyz^⋅−)₄]‧10THF (Ln = Gd (3), Dy (4)) complexes. Magnetic and computational studies reveal one of the highest exchange couplings (J_Gd-pyz = −22.2 cm⁻¹) for a radical-bridged system, achieved by two 4f-SOMO interactions. This, combined with the significant anisotropy of the Dy^III, grants 2 and 4 with slow magnetic relaxation at zero field and open hysteresis loops. A giant coercive field of 65 kOe renders 4 as the hardest radical-bridged Dy-based SMM.

现代生活方式与使用永磁体的技术成就交织在一起。多核镧系元素单分子磁体 (SMM) 缺乏强磁通信，这使得高性能 SMM 的设计成为持续的挑战。为了克服这个问题，在镧系元素之间掺入自由基吡嗪 (pyz ^⋅− ) 连接体是一种引人注目的方法。仔细调整合成条件导致双核 [(Cp* ₂ Ln ^III ) ₂ (pyz ^⋅− )(THF) ₂ ][BPh ₄ ] (Ln = Gd ( 1 ), Dy ( 2 ); Cp* = 五甲基环戊二烯基； THF = 四氢呋喃）和四核 [(Cp* ₂ Ln ^III ) ₄ (pyz ^⋅− ) ₄ ]‧10THF (Ln = Gd ( 3 ), Dy ( 4 )) 配合物。磁性和计算研究揭示了自由基桥接系统的最高交换耦合之一（J _Gd-pyz  = -22.2 cm ^{-1 ），通过两个 4} f -SOMO 相互作用实现。这与 Dy ^III的显着各向异性相结合，使2和4在零场和开磁滞回线下具有缓慢的磁弛豫。 65 kOe 的巨大矫顽力场使4成为最硬的自由基桥接镝基 SMM。