High Performance 2D Conductive Magnets through Redox Active Coordination Chemistry – HiPerMagnet

The HiPerMagnet project consists in the preparation and characterization of novel magnetically ordered and conductive 2D coordination polymers with tunable properties using the versatility of the molecular chemistry. The materials will contain redox-active ligands and metal ions having high reducing redox ability. The objectives are to promote electron transfer between the metal ions and the ligands or, if the redox process is disabled or partial in the final material, to generate organic radicals through post-synthetic reduction. We hope to obtained new molecule-based materials possessing high conductivity and ferro-, ferri- or antiferromagnetic states at high temperature. The 2D materials will also be exfoliated and introduced as single layers in spintronics devices. Within our project, we want to be able to answer several questions facing the molecular materials research field and the physical chemistry community,
(i) How can we synthesize molecule-based compounds with magnetically ordered phases (ferro/ferri or antiferro) at high temperature?
(ii) How can we design molecule-based systems with tunable band gaps and carrier densities in order to promote high electrical conductivity?
(iii) How can we prepare molecule-based magnetic semiconductors that work at room temperature?
(iv)vCan we make molecule-based spintronic devices showing exotic states at low temperatures?
(v) Can we make spintronic molecule-based devices working at room temperatures?


To reach our goals, the proposed project gathers during 48 months four partners: the M3 team of the CRPP (P1), the SMM group of ICMCB (P2) at Pessac, the ID12 team at ESRF (P3), and QuantECA group at Néel Institute (P4) at Grenoble. We want to recruit 2 post-docs to help us in our projet.

Our ambitious goals will be fulfilled by the engineering of the electronic structure of 2D coordination polymers, ie. by matching the energy levels of the inorganic (3d metal ions) and organic (redox active ligands) building blocks to give rise to strong electron mobility and strong magnetic interactions.
The first part of this project will be devoted to the fine tuning of the p- and d-orbital energies of the ligands and metal ions of different electronic configurations, to promote the redox process, and subsequent radical ligand formation as observed in our recent work published in Nature Chemistry for the 2D compound [Cr(pyrazine)2Cl2], which constitutes our proof-of-concept. In the cases for which an optimal orbital overlap is not achieved and thus the redox process is disabled or is only partial, radical ligands will be generated by post-synthetic methods in the second part of our project. It is known that the post-synthetic chemical reduction by means of reducing agents, such as alkali metal salts or cobaltocene, has already yielded record Tc values for magnetic order, as well as highly conductive Metal Organic Frameworks. Finally, in the third part the most promising 2D CPs will be exfoliated into single layer nanoflakes and the high-quality films will be incorporated into three different devices. The gate doping at the single-layer level will provide us with a microscopic picture on the interaction between the delocalized electrons in the p ligands and the magnetic moment localized on the metal centres and will give insights into the potential implementation of 2D CPs in spintronic devices.