Abstract

We report a 35^{35}Cl nuclear magnetic resonance (NMR) study of the diluted Kitaev material αα-Ru1−x_{1-x}Irx_xCl3_3 (x=0.1x=0.1 and 0.20.2) where non-magnetic Ir3+^{3+} dopants substitute Ru3+^{3+} ions. Upon dilution, the 35^{35}Cl spectra exhibit unusual large magnetic inhomogeneity, which sets in at temperatures below the Kitaev exchange energy scale. At the same time, the 35^{35}Cl spin-lattice relaxation rate T1−1T_1^{-1} as a function of dilution and magnetic field unravels a critical doping of xc≈0.22x_c\approx 0.22, towards which both the field-induced spin gap and the zero-field magnetic ordering are simultaneously suppressed, while novel gapless low-energy spin excitations dominate the relaxation process. These NMR findings point to the stabilization of a random singlet phase in αα-Ru1−x_{1-x}Irx_xCl3_3, arising from the interplay of dilution and exchange frustration in the quantum limit.

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