Enhancing single-molecule magnet behavior of linear CoII-DyIIICoII complex by introducing bulky diamagnetic moiety

Single-molecule magnets (SMMs) are regarded as promising candidates for ultrahigh-density storage, quantum information processing and molecular spintronics. It is a crucial challenge for chemists to modulate magnetic dynamics of SMMs. Here, we successfully synthesized two 3d-4f polynuclear compounds [Co2Dy(TTTTCl)2(MeOH)]NO3·3MeOH (1) and [Co2Dy(TTTTCl)2 (MeOH)][Co(HTTTTCl)](NO3)2·2.5MeOH·2H2O (2), where H3TTTTCl=2,2′,2′′-(((nitrilotris(ethane-2,1-diyl)) tris(azanediyl)) tris(methylene))tris-(4-chlorophenol). On applying the approach by co-crystallization of bulky diamagnetic moiety, the effective energy barrier enhances from 401 K (1) to 536 K (2), which are both among the highest d-f heterometallic SMMs.