Abstract
The effects of external pressure on a high-performing dysprosocenium single-molecule magnet are investigated using a combination of X-ray diffraction, magnetometry and theoretical calculations. The effective energy barrier (U(eff)) decreases from ca. 1300 cm(-1) at ambient pressure to ca. 1125 cm(-1) at 3 GPa. Our results indicate that compression < 1.2 GPa has a negligible effect on the Orbach process, but magnetic relaxation > 1 GPa increases via Raman relaxation and/or quantum tunnelling of magnetisation.