Solvatotuning of the Field-Induced Slow Magnetic Relaxation through a Single-Crystal-to-Single-Crystal Transformation in Pentanuclear Gadolinium(III)-Nickel(II) Complexes

The partial loss of crystallization water molecules in the gadolinium(III)-nickel(II) dithiooxalate dodecahydrate [Gd2Ni3(dto)6(H2O)10]·12H2O (1) to yield dihydrate derivative [Gd2Ni3(dto)6(H2O)10]·2H2O (2) provokes significant and reversible changes spin relaxation dynamics. This unique single-crystal-to-single-crystal transformation emerges as a new route toward solvatoswitchable single-molecule magnets for molecular spintronics quantum computing.