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RESEARCH PRODUCT

Chemical Design and Magnetic Ordering in Thin Layers of 2D Metal–Organic Frameworks (MOFs)

Iñigo J. Vitorica-yrezabalMartin LeeSamuel Mañas‐valeroJavier López-cabrellesHerre S. J. Van Der ZantGuillermo Mínguez EspallargasEugenio CoronadoPeter G. SteenekenMakars ŠIškins

subject

FabricationThin layersChemistryQuímica organometàl·lica02 engineering and technologyGeneral Chemistry010402 general chemistry021001 nanoscience & nanotechnology01 natural sciencesBiochemistryCatalysisArticle0104 chemical sciencesCrystallinitysymbols.namesakeColloid and Surface ChemistryChemical physicsMagnetsymbolsMoleculeMetal-organic frameworkvan der Waals force0210 nano-technologyMaterialsTopology (chemistry)

description

Through rational chemical design, and thanks to the hybrid nature of metal−organic frameworks (MOFs), it is possible to prepare molecule-based 2D magnetic materials stable at ambient conditions. Here, we illustrate the versatility of this approach by changing both the metallic nodes and the ligands in a family of layered MOFs that allows the tuning of their magnetic properties. Specifically, the reaction of benzimidazole-type ligands with different metal centers (MII = Fe, Co, Mn, Zn) in a solventfree synthesis produces a family of crystalline materials, denoted as MUV-1(M), which order antiferromagnetically with critical temperatures that depend on M. Furthermore, the incorporation of additional substituents in the ligand results in a novel system, denoted as MUV-8, formed by covalently bound magnetic double layers interconnected by van der Waals interactions, a topology that is very rare in the field of 2D materials and unprecedented for 2D magnets. These layered materials are robust enough to be mechanically exfoliated down to a few layers with large lateral dimensions. Finally, the robustness and crystallinity of these layered MOFs allow the fabrication of nanomechanical resonators that can be used to detect-through laser interferometry-the magnetic order in thin layers of these 2D molecule-based antiferromagnets.

10.1021/jacs.1c07802http://dx.doi.org/10.1021/jacs.1c07802