Historically, solid-state materials dominated the development of new magnetic technologies. The use of permanent magnets such as Neodymium Iron Boride (NdFeB) and Samarium Cobalt (SmCo) in computer disc drives and car batteries underpinned much of this progress. Recent interest in metal-organic-magnets (MOMs) as designer magnets has emerged as a result of the synthetic modularity and chemical diversity of their building blocks. This tunability can also be exploited in the development of materials with novel spin physics, such as spin frustrated behavior and unconventional magnetic order. Towards this end, this research highlights two strategies: (1) designing two-dimensional (2D) MOMs with two competing nearest-neighbor spin interaction pathways (J1 and J2) to engender spin frustrated behavior and (2) creating a series of chemically similar but dimensionally distinct MOMs to investigate the effect of dimensionality on magnet behavior. In the first project, we introduce a new class of 2D S = ½ Cu2+- or S = 1 Ni2+- based J1/J2 magnets and discuss how magnet topology and the magnitude of J1/J2 influence the realization of exotic ground-states. For the second project, we demonstrate the use of synthetic chemistry to controllably build up spin interactions in a series of S = 1 Ni2+ oxalate-based MOMs. A new candidate Haldane spin chain will be introduced in addition to experimental realization of unconventional magnetic order in its higher dimensional spin analogues. These results demonstrate how we harness synthetic chemistry to create bespoke magnetic materials with novel spin physics.

Unconventional spin physics in designer metal-organic magnets

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