Approaching the uniaxiality of magnetic anisotropy in singlemolecule magnets

Single-molecule magnets(SMMs),which can exhibit slow magnetization relaxation and bulk-magnet-like hysteresis of purely molecular origin,are promising candidates for high-density information storage,molecular spintronics,and quantum computing.To realize their applications,it is crucial to improve the blocking temperature(TB)and the effective relaxation barrier(Ueff).Three decades of multidisciplinary research have yielded distinct SMMs with a state-of-the-art Ueff of up to 2,000 K and a TB of up to the liquid nitrogen region.Several strategies have been investigated and summarized,which revealed that enhancing the uniaxiality of magnetic anisotropy is critical for constructing high-performance SMMs.Therefore,magnetic anisotropy,a key property that connects the molecular structure symmetry and performance of SMMs,plays a fundamental role in dictating magneto-structural correlations.Understanding and employing magnetic anisotropy would be significantly beneficial for rationally designing high-performance SMMs.This review focuses on the magnetic anisotropy of SMMs.We illustrate the origin and manifestation of magnetic anisotropy in mononuclear 3d-and 4f-block metal complexes.We then introduce developed approaches to investigate magnetic anisotropy both theoretically and experimentally.Typical SMMs by optimizing uniaxial magnetic anisotropy through lanthanide metallocene,symmetry controlling,and low-coordination approaches are represented.Furthermore,the remaining challenges and opportunities in this field will be discussed.