Pressure-driven high-to-low spin transition in the bimetallic quantum magnet [Ru2(O2 CMe)4]3[Cr(CN)6]

Synchrotron-based infrared and Raman spectroscopies were brought together with diamond anvil cell techniques and an analysis of the magnetic properties to investigate the pressure-induced high → low spin transition in [Ru2(O2CMe)4]3[Cr(CN)6]. The extended nature of the diruthenium wave function combined with coupling to chromium-related local lattice distortions changes the relative energies of the π∗ and δ∗ orbitals and drives the high → low spin transition on the mixed-valence diruthenium complex. This is a rare example of an externally controlled metamagnetic transition in which both spin-orbit and spin-lattice interactions contribute to the mechanism.