Spin–Lattice Coupling Across the Magnetic Quantum-Phase Transition in Copper-Containing Coordination Polymers

We measured the infrared vibrational properties of two copper-containing coordination polymers, [Cu(pyz)2(2-HOpy)2](PF6)2 and [Cu(pyz)1.5(4-HOpy)2](ClO4)2, under different external stimuli in order to explore the microscopic aspects of spin–lattice coupling. While the temperature and pressure control hydrogen bonding, an applied field drives these materials from the antiferromagnetic → fully saturated state. Analysis of the pyrazine (pyz)-related vibrational modes across the magnetic quantum-phase transition provides a superb local probe of magnetoelastic coupling because the pyz ligand functions as the primary exchange pathway and is present in both systems. Strikingly, the PF6– compound employs several pyz-related distortions in support of the magnetically driven transition, whereas the ClO4– system requires only a single out-of-plane pyz bending mode. Bringing these findings together with magnetoinfrared spectra from other copper complexes reveals spin–lattice coupling across the magnetic quantum-phase...