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Collective excitations in the tetravalent lanthanide honeycomb antiferromagnet Na2PrO3

M. J. Daum1,*, A. Ramanathan2,*, A. I. Kolesnikov3, S. Calder3, M. Mourigal1,†, and H. S. La Pierre2,4,‡

  • 1School of Physics, Georgia Institute of Technology, Atlanta, Georgia 30332, USA
  • 2School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia 30332, USA
  • 3Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
  • 4Nuclear and Radiological Engineering and Medical Physics Program, School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332, USA

  • *These authors contributed equally to this work.
  • †mourigal@gatech.edu
  • ‡hsl@gatech.edu

Phys. Rev. B 103, L121109 – Published 12 March, 2021

DOI: https://doi.org/10.1103/PhysRevB.103.L121109

Abstract

Thermomagnetic and inelastic neutron-scattering measurements on Na2PrO3 are reported. This material is an antiferromagnetic honeycomb magnet based on the tetravalent lanthanide Pr4+ and has been proposed to host dominant antiferromagnetic Kitaev interactions. These measurements reveal magnetic fluctuations in Na2PrO3 below an energy of 2 meV as well as crystal-field excitations around 230 meV. The latter energy is comparable to the scale of the spin-orbit interaction and explains both the very small effective moment of around 1.0μB per Pr4+ and the difficulty to uncover any static magnetic scattering below the ordering transition at TN= 4.6 K. By comparing the low-energy magnetic excitations in Na2PrO3 to those of the isostructural spin-only compound, Na2TbO3, a microscopic model of exchange interactions is developed that implicates dominant and surprisingly large Heisenberg exchange interactions J≈1.1(1) meV. Although antiferromagnetic Kitaev interactions with K≤0.2J cannot be excluded, the inelastic neutron-scattering data of Na2PrO3 is best explained with a Δ=1.22 easy-axis XXZ exchange anisotropy.

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