A novel Gapless Quantum Spin Liquid in the S = 1 4d4-honeycomb material Cu${}_3$LiRu${}_2$O${}_6$

Abstract

We report the discovery of a novel gapless quantum spin liquid in the S=1 honeycomb system Cu${}_3$LiRu${}_2$O${}_6$ with Ru${}^{4+}$ ($4d^4$) where moments remain dynamic down to 50 mK. Heat capacity measurements show no sign of magnetic ordering down to 60 mK in spite of a Curie-Weiss temperature = -222 K indicating a strong antiferromagnetic interaction. In zero field, magnetic heat capacity shows a linear T-dependence with Sommerfeld coefficient = 107 mJ/mol K${}^2$ is much larger than that found in typical Fermi liquids. Our local probe ${}^7$Li nuclear magnetic resonance (NMR) measurements find a significant temperature-independent ${}^7$Li NMR shift (and hence a non-zero spin susceptibility) at low-T and a linear T-variation of the ${}^7$Li NMR spin-lattice relaxation rate 1/T${}_1$ at low-T reminiscent of fermionic excitations. Muon spin relaxation measurements detect neither long-range ordering nor spin freezing down to 50 mK and the temperature variation of the muon depolarization rate shows a gradual increase with decreasing temperature and a leveling off below about 1 K evincing a persistent spin dynamics common to several spin liquid candidates. Our results provide strong signatures of a quantum spin liquid in the titled honeycomb material.

5 pages and 6 figures in main, 8 pages and 16 figures in the supplement. arXiv admin note: text overlap with arXiv:2405.06380