Multifunctional molecules that respond both to magnetic fields and light are subject of study due to possible applications in fields as diverse as imaging or information processing and storage. In this paper we report visible and NIR emitting single-molecule magnets (SMMs) of Yb(III) and Er(III) with symmetric (SYML) and asymmetric (AZOL) Schiff base ligands. The prepared complexes SYML–Ln2 and AZOL–Ln3 (Ln = Er, Yb) are SMMs, with the exception of AZOL–Yb3, with a relaxation behavior dominated by quantum tunneling of magnetization. The multi-level double-decker structure of the complexes is ideal for surface deposition in carbon-based materials.
