Collective excitations in the tetravalent lanthanide honeycomb antiferromagnet Na2Pr O3

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.