<p>Molecular frameworks with ReO<sub>3</sub>- 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)<sub>3</sub>, a three-dimensional molecular framework adopting a cubic ReO<sub>3</sub>-type structure, in which Cr<sup>3+</sup> ions are bridged exclusively by pyrazine radical anions. In Cr(pyrazine)<sub>3</sub>, antiferromagnetic coupling between the Cr<sup>3+</sup> 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)<sub>3</sub> among the very few materials featuring robust compensated ferrimagnetism under ambient conditions.</p><p></p>

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

  • Frédéric Aribot,
  • Maja A. Dunstan,
  • Nathan J. Yutronkie,
  • Mariusz Kubus,
  • Luis Leyva-Parra,
  • Anton Viborg,
  • Susanne Mossin,
  • Fabrice Wilhelm,
  • Vivian Nassif,
  • Dawid Pinkowicz,
  • Wiktor Wolański,
  • Lukas B. Woodcock,
  • Stergios Piligkos,
  • Jesper Bendix,
  • Sebastian E. Reyes-Lillo,
  • Andrei Rogalev,
  • Kasper S. Pedersen

摘要

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.