Tuning the magnetic properties of 2D molecule-based magnets via rational control of the layer-layer distance

In our group’s efforts toward high-temperature molecule-based magnets, we have recently reported the network Li0.7[Cr(pyrazine)2]Cl0.7∙0.25(THF) (THF = tetrahydrofuran), which features ferrimagnetic order up to a ground-breaking critical temperature of 515 K. It is the aim of this project to further our understanding of this network by examining the effect of substituting Li+ in the synthesis for other alkali metal cations (Na+, K+, Rb+, and Cs+). We seek to probe the physical, electronic, and magnetic structure in these compounds via X-ray absorption near edge structure (XANES), X-ray magnetic circular dichroism (XMCD), and high-resolution powder X-ray diffraction (HR-PXRD). Elucidating the effects of the alkali metal on the magnetic hysteresis, Tc, layer-layer distance, and other properties will extend our ability to rationally design 2D networks toward desired properties, paving the way for new and improved molecule-based magnets for applications in next-generation devices.