Spin-lattice interactions as revealed by the pressure-temperature phase diagram of Co[N(CN)2]2

We combined diamond anvil cell techniques, synchrotron-based infrared and Raman spectroscopies, and complementary lattice dynamics calculations to investigate spin-lattice coupling and the magnetic crossover mechanism in the molecule-based quantum magnet Co[N(CN)2]2. These findings along with prior magnetic properties work were brought together to create a pressure-temperature phase diagram in which the second-order structural boundaries converge on key areas of activity involving the spin state, exposing how the pressure-induced local lattice distortions trigger the ferromagnetic to antiferromagnetic crossover transition. Similar triggering events may take place in other materials.