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Contrasting structural reversibility and magnetic correlations in isostructural honeycomb magnets CrCl3 and α−RuCl3

Zachary Morgan1,*, Iris Ye2, Jiasen Guo1, Michael A. McGuire3, and Jiaqiang Yan3

  • *Contact author: morganzj@ornl.gov
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Phys. Rev. Materials 10, 094001 – Published 3 September, 2026

DOI: https://doi.org/10.1103/33fq-c8cr

Abstract

We report a comparative neutron single crystal diffraction study of the structural and magnetic properties of layered halides CrCl3 and α−RuCl3. They host a honeycomb arrangement of transition metal ions with distinct electronic configurations and undergo a first-order structural transition between high-temperature C2/m and low-temperature R3¯. Both compounds show a step-like change in the c-lattice parameter across the structure transition. In contrast, the in-plane lattice response is quite different: α−RuCl3 exhibits an abrupt hysteretic change across the transition accompanied by progressive crystalline degradation upon thermal cycling, whereas CrCl3 shows a smooth in-plane lattice evolution and remains structurally robust. Magnetically, CrCl3 orders into an A-type antiferromagnetic structure at TN=14 K and exhibits pronounced diffuse magnetic scattering extending up to about 40 K. α−RuCl3 shows no observable magnetic diffuse scattering above its zigzag antiferromagnetic ordering temperature TN=7.6 K. These results suggest that the contrasting structural responses arise from an interplay between interlayer sliding energetics, stacking-strain coupling, and elastic accommodation of the stacking transition. The distinct chemical bonding and electronic configurations of the two compounds provide a microscopic basis for their different lattice responses to the structure transition and magnetic correlations.

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Phys. Rev. Materials 10, 094001– Published 3 September, 2026
  • Received 21 May 2026
  • Accepted 4 August 2026
Article part of CHORUS
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