Phase behavior and electronic properties of a conducting ferrimagnetic metal-organic framework from first principles*

Metal–organic frameworks (MOFs) are an emerging class of readily-tunable three-dimensional porous materials consisting of periodic arrays of metal cations connected by organic ligands. Most MOFs are insulating and nonmagnetic. CrCl2(pyrazine)2 [1] is a quasi-two-dimensional layered MOF with ferrimagnetic ordering below 55 K and a comparably large conductivity of 32 mS/cm at room temperature. Here, we perform first principles density functional theory calculations to understand the low temperature electronic, vibrational, and magnetic properties of CrCl2(pyrazine)2 at equilibrium and under compression, comparing with recent measurements of trends in structure and conductivity up to 15 GPa.
[1] Pederson et al. Nature Chemistry volume 10, pages1056–1061(2018)