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Structure transition and zigzag magnetic order in Ir/Rh-substituted honeycomb lattice α−RuCl3

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Physical Review Materials
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We report magnetization and neutron diffraction studies on crystal and magnetic structures of Ir- and Rh-substituted honeycomb lattice α−RuCl3. The iridium or rhodium atoms are distributed at the Ru site with little structural modification. Both systems undergo a room-temperature monoclinic C2/m to low-temperature trigonal R¯3 phase transformation with a large recoverable hysteresis. At low temperature, a zigzag spin order is observed with the same characteristic wave vector (0,0.5,1) as in the parent α−RuCl3. Detailed magnetic structure refinement reveals an ordered moment of 0.32(5)µB/Ru and an upper boundary of canting angle of 15(4)∘ away from the basal plane at 5 K for the 10% Ir-substituted α−RuCl3, which is different from the 0.45–0.73 µB/Ru and 32∘–48∘ canting angle reported in the parent compound α−RuCl3. The observation of unchanged RuCl6 local octahedral environment, reduced ordered magnetic moment size and canting angle compared to previously reported highlights the potential to study quantum spin-liquid behavior through nonmagnetic ion doping.