LAUSR

It is challenging to use achiral ligands to spontaneously construct chiral molecular magnets. In this work, two new Ln4 cluster complexes based on N,N′-(1,3-propanediyl)bis[N-[1,1-bis(hydroxymethyl)-2-hydroxyethyl]amine] (H6L) have been assembled, which are crystallized in a chiral space group due to the asymmetric distribution of acetate (OAc–) groups and hexafluoroacetylacetonate (F6acac–) groups on both sides of the parallelogram-like Ln4 core. Complex 1, [Dy4(H3L)2(OAc)3(F6acac)3]·5MeOH·2H2O, exhibits single-molecule magnet properties at the zero field with the Ueff/k value of 48.4 K; notably, besides the Orbach process, the Raman process is also prominent for the magnetic relaxation of 1. Complex 2, [Gd4(H3L)2(OAc)3(F6acac)3]·4MeOH·2.5H2O, displays a large magnetocaloric effect, whose largest −ΔSm value is 21.88 J kg–1 K–1 (when T = 2 K and ΔH = 5 T); it thus can be utilized as a good magnetic refrigeration molecular material.