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 (Ueff) decreases from ca. 1300 cm−1 at ambient pressure to ca. 1125 cm−1 at 3 GPa. Our results indicate that compression 1 GPa increases via Raman relaxation and/or quantum tunnelling of magnetisation.
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