Dilution of the Magnetic Lattice in the Kitaev Candidate Α−rucl3 by Rh3+ Doping

Magnetic dilution of a well-established Kitaev candidate system is realized in the substitutional Ru1-xRhxCl3 series (x = 0.02-0.6). Optimized syntheses protocols yield uniformly doped single crystals and polycrystalline powders that are isostructural to the parental alpha-RuCl3 as per x-ray diffraction. The Rh content x is accurately determined by the quantitative energy-dispersive x-ray spectroscopy technique with standards. We determine the magnetic phase diagram of Ru1-xRhxCl3 for in-plane magnetic fields from magnetization and specific-heat measurements as a function of x and stacking periodicity and identify the suppression of the magnetic order at x approximate to 0.2 towards a disordered phase, which does not show any clear signature of freezing into a spin glass. Comparing with previous studies on the substitution series Ru1-xRhxCl3, we propose that chemical pressure would contribute to the suppression of magnetic order, especially in Ru1-xRhxCl3, and that the zigzag magnetic ground state appears to be relatively robust with respect to the dilution of the Kitaev-Gamma-Heisenberg magnetic lattice. We also discovered a slight dependence of the magnetic properties on thermal cycling, which would be due to an incomplete structural transition.