Nanostructuring of Rare-earth-based Single-Molecule Magnets as Long-range Ordered Arrays in the Framework of Organic Metal Halide Perovskites

The nanostructuring of single-molecule magnets (SMMs) on substrates, in nanotubes and periodic frameworks is highly desired for the future magnetic recording devices. However, the ability to organize SMMs into long-range ordered arrays in these systems is still lacking. Here, we report the incorporation of magnetic (RECl₂ (H₂ O)₆ )⁺ (RE=rare earths) molecular groups into the framework of an organic metal halide perovskite (OMHP)-(H₂ dabco)CsCl₃ . Intriguingly, we show the incorporated rare-earth groups self-organized into long-range ordered arrays that uniformly and periodically distributed in the A sites of OMHP. The ordered (RECl₂ (H₂ O)₆ )⁺ groups serve as SMMs in the perovskite frameworks, exhibiting large effective magnetic moment, moderate magnetic anisotropy and two-step relaxation behavior. With the additional merit of great structural flexibility and multifunction of OMHPs, the preparation of the first SMMs@OMHP magnetic materials furthers the development of molecular spintronics.