We report the synthesis, structure and magnetic investigations of two new Dy3+ homoleptic ate-complexes based on different ene-diamido ligands [K(THF)2][Dy(DAD2R)2] (R = H (1), Me (2) DAD2R = [2,6-iPr2C6H3N–CR![[double bond, length as m-dash]](http://www.rsc.org/images/entities/char_e001.gif)
CR–NC6H3iPr2-2,6] showing K+/arene interactions. Magnetic investigations reval that both compounds exhibit a zero-field single-molecule magnetic relaxation mainly governed by a Raman process.
