Persistence of antiferromagnetic order upon La substitution in the 4d 4 Mott insulator Ca 2 RuO 4
2018
The chemical and magnetic structures of the series of compounds Ca2−xLaxRuO4 [x = 0, 0.05(1), 0.07(1), 0.12(1)] have been investigated using neutron diffraction and resonant elastic x-ray scattering. Upon La doping, the low-temperature S-Pbca space group of the parent compound is retained in all insulating samples [x ≤ 0.07(1)], but with significant changes to the atomic positions within the unit cell. These changes can be characterized in terms of the local RuO6 octahedral coordination: with increasing doping, the structure, crudely speaking, evolves from an orthorhombic unit cell with compressed octahedra to a quasitetragonal unit cell with elongated ones. The magnetic structure on the other hand, is found to be robust, with the basic k = (0,0,0), b-axis antiferromagnetic order of the parent compound preserved below the critical La doping concentration of x ≈ 0.11. The only effects of La doping on the magnetic structure are to suppress the A-centred mode, favoring the B mode instead, and to reduce the Neel temperature somewhat. Our results are discussed with reference to previous experimental reports on the effects of cation substitution on the d4 Mott insulator Ca2RuO4, as well as with regard to theoretical studies on the evolution of its electronic and magnetic structure. In particular, our results rule out the presence of a proposed ferromagnetic phase, and suggest that the structural effects associated with La substitution play an important role in the physics of the system.
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