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Persistent compensated ferrimagnetism in the molecular framework Cr(pyrazine)3

Nature Chemistry (2026)Cite this article

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Abstract

Molecular frameworks with ReO3- or perovskite-related topologies have been widely investigated for their structural versatility, yet examples displaying strong electronic and magnetic correlations have not been realized in such systems. Here we report the synthesis of Cr(pyrazine)3, a three-dimensional molecular framework adopting a cubic ReO3-type structure, in which Cr3+ ions are bridged exclusively by pyrazine radical anions. In Cr(pyrazine)3, antiferromagnetic coupling between the Cr3+ and radical sublattices, comparable in magnitude to that found in transition-metal oxides, leads to a nearly perfectly compensated ferrimagnetic ground state with an exceptionally small net magnetic moment. Owing to the symmetry and stoichiometry of the bipartite lattice, magnetic compensation persists over an extended temperature range rather than occurring only at a specific compensation temperature. Long-range magnetic order is observed well above room temperature, placing Cr(pyrazine)3 among the very few materials featuring robust compensated ferrimagnetism under ambient conditions.

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Fig. 1: Structure of Cr(pyz)3.
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Fig. 2: X-ray absorption spectroscopy.
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Fig. 3: Magnetic properties of Cr(pyz)3.
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Data availability

All data are available in the main text, the Supplementary Information and in the Source Data files provided with this Paper. Crystallographic data for the structures reported in this Article have been deposited at the Cambridge Crystallographic Data Centre, under deposition nos. CCDC 2487374 (250 K) and 2487375 (120 K). Copies of the data can be obtained free of charge via https://www.ccdc.cam.ac.uk/structures/. Source data are provided with this Paper.

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Acknowledgements

K.S.P. thanks the Villum Foundation for a VILLUM Young Investigator grant and a VILLUM Young Investigator+ (42094) grant, the Independent Research Fund Denmark for a DFF-Sapere Aude Starting Grant (0165-00073B), and the Carlsberg Foundation for a research infrastructure grant (CF17-0637). This work was supported by the Danish National Committee for Research Infrastructure (NUFI) through the ESS-Lighthouse Q-MAT. S.E.R.-L. acknowledges ANID Fondecyt grant no. 1220986. L.L.-P. was funded by the Postdoctoral Talent Attraction Competition for Research Centers and Institutes of the Universidad Andres Bello (UNAB) 2025, project no. DI-02-25/ATP. Powered@NLHPC research was partially supported by the supercomputing infrastructure of the NLHPC (CCSS210001). D.P. acknowledges financial support from the European Union within the Horizon Europe Framework Programme via ERC Consolidator Grant LUX-INVENTA (101045004). We acknowledge the Copenhagen Pulse-EPR Facility, financed by research grant NNF21OC0068806 Research Infrastructure – Large Equipment and Facilities 2021 from the Novo Nordisk Foundation. The X-ray spectroscopy experiments were performed at the ID12 beamline at the European Synchrotron Radiation Facility (Grenoble, France)67. Neutron diffraction experiments were performed at Institut Laue-Langevin (Grenoble, France)68. We thank the Technical University of Denmark for funding the DTU Electron Crystallography Facility, and the Danish Agency for Science, Technology, and Innovation for funding the instrument centre ‘Danscatt’.

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  1. These authors contributed equally: Frédéric Aribot, Maja A. Dunstan.

Authors and Affiliations

  1. Department of Chemistry, Technical University of Denmark, Lyngby, Denmark

    Frédéric Aribot, Maja A. Dunstan, Mariusz Kubus, Anton Viborg, Susanne Mossin & Kasper S. Pedersen

  2. ESRF – The European Synchrotron, Grenoble, France

    Nathan J. Yutronkie, Fabrice Wilhelm & Andrei Rogalev

  3. Centro de Investigación para el Diseño de Materiales (CEDEM), Facultad de Ciencias Exactas, Departamento de Ciencias Químicas, Universidad Andres Bello, Santiago, Chile

    Luis Leyva-Parra

  4. Institut Laue-Langevin, Grenoble, France

    Vivian Nassif

  5. Institut Néel, Université Grenoble Alpes, Grenoble, France

    Vivian Nassif

  6. Faculty of Chemistry, Jagiellonian University, Kraków, Poland

    Dawid Pinkowicz & Wiktor Wolański

  7. Department of Chemistry, University of Copenhagen, Copenhagen, Denmark

    Lukas B. Woodcock, Stergios Piligkos & Jesper Bendix

  8. Departamento de Física y Astronomía, Universidad Andres Bello, Santiago, Chile

    Sebastian E. Reyes-Lillo

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  1. Frédéric Aribot
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Contributions

K.S.P. conceived and supervised the project. F.A. synthesized and chemically characterized the material. F.A., M.A.D. and M.K. performed the powder and single-crystal X-ray crystallographic analysis. K.S.P. and F.A. performed the magnetometry studies. N.J.Y., F.W., A.R., M.A.D., A.V., F.A. and K.S.P. performed and analysed the XAS experiments. D.P. obtained and analysed the differential scanning calorimetry data. D.P. and W.W. obtained and analysed the photomagnetization data. L.L.-P., S.E.R.-L. and J.B. performed the DFT computational studies. L.B.W., S.P. and S.M. obtained the EPR spectroscopic data. V.N., M.A.D., K.S.P. and M.K. obtained and analysed the neutron powder diffractograms. The manuscript was written by K.S.P., M.A.D. and F.A. through contributions from all authors. All authors have consented to publication of the manuscript.

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Correspondence to Kasper S. Pedersen.

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Atomic coordinates used for DFT calculations.

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X-ray absorption spectroscopy data.

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Magnetization data.

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Aribot, F., Dunstan, M.A., Yutronkie, N.J. et al. Persistent compensated ferrimagnetism in the molecular framework Cr(pyrazine)3. Nat. Chem. (2026). https://doi.org/10.1038/s41557-026-02131-8

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