Enhancing blocking temperature using inverse hydrogen bonds for non-radical bridged dimeric Dy(III) single-molecule magnets

Single-molecule magnets (SMMs) are a kind of nanosized magnetic materials that are capable of storing massive bytes of information. Strongly coupling the spin centers in a proper manner is a usual approach to promote the working temperature (or blocking temperature) for SMMs. Electron delocalized radicals have been widely employed to accomplish this job. Here, we show a new manner by using weak but multiple B–H^δ− ⋯ Dy³⁺ inverse hydrogen bonding (IHB) interactions to control the magnetic couplings in a series of dimeric dysprosiacaborane SMMs. This approach leads to a record high T_B^100s of 10 K among non-radical bridged dimeric SMMs, which is mainly ascribed to strong ferromagnetic coupling (4.38 cm⁻¹) and the proper alignment of the magnetic principle axes of the adjacent dysprosium(III) ions. In verifying by theoretical calculations, these results demonstrate that IHB interactions can be used to construct strong axial ferromagnetic coupling and enhancing magnetic blocking temperature for SMMs.