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Controlled formation of desired lanthanide supramolecular complexes is challenging because of the difficulties in predicting coordination geometry, as well as a labile coordination number. Herein, we explore the effect of ionic radii and linker length on supramolecular species formation. A helicate-to-tetrahedron transformation occurred between [Ln 2  L1  3 ] and [Ln 4  L1  6 ] (Ln = La, Sm, Eu, Gd, Tb and Lu). For six lanthanide ions, the unfavored tetrahedron [La 4  L1  6 ] can only be observed in a concentrated mixture with the helicate [La 2  L1  3 ] where no pure [La 4  L1  6 ] species was isolated via crystallization. For Sm, Eu, Gd, Tb, the [Ln 4  L1  6 ] supramolecular tetrahedron can be isolated via crystallization from diisopropyl ether. A similar result was also observed for Lu, but the tetrahedral structure was found to be relatively stable and transformed back to [Lu 2  L1  3 ] much slower upon dissolution.  No tetrahedron formation was observed with  L3  giving rise to only [Ln 2  L3  3 ] species, in which  L3  contains a longer and more flexible linker compared with that of  L1 . Results show that the supramolecular transformation in these systems is governed by both the ionic radii as well as the ligand design. Special focus is on both [Eu 2  L1  3 ] and [Eu 4  L1  6 ] which form chiral entities and exhibit interesting circular polarized luminescence.

Helicate-to-tetrahedron transformation of chiral lanthanide supramolecular complexes induced by ionic radii effect and linker length