From Molecules to Frustrated Networks: Investigating Magnetic Interactions

Molecule-based frameworks represent a cutting-edge synthetic approach for designing spin-frustrated magnets, offering a powerful route to self-assembled materials that could unlock exotic phenomena such as quantum spin liquids (QSL). Here, we present a triangular discrete system, [Cr3(HAN)(MeCN)12](PF6)6 (1), with potential as frustrated building block that can be further extended into high-dimensional systems [Cr(HAN)] (2). To ensure magnetic frustration within the metal centers, engineering of the metal-ligand interaction is crucial. We are focused on efficiently controlling the interaction between the magnetic centers through successive post-synthetic reductions to achieve frustration. In this context, we propose using XANES, EXAFS, and XMCD measurements at ID12 to probe the local electronic structures of the Cr centers. These techniques will provide invaluable insights into the electronic structure of this molecule and help elucidate the role of metal-ligand interaction.