High pressure sequence of Ba_3NiSb_2O_9 structural phases: new S=1S = 1 quantum spin-liquids based on Ni^{2+}

preprint2011arXivOpen access

Abstract

By using a high pressure, high temperature (HPHT) technique, the antiferromagnetically ordered (TNT_N = 13.5 K) 6H-A phase of Ba3_3NiSb2_2O9_9 was transformed into two new gapless quantum spin liquid(QSL) candidates with S=1 (Ni2+^{2+}) moments: the 6H-B phase with a Ni2+^{2+}-triangular lattice and the 3C-phase with a Ni2+^{2+}-three-dimensional (3D) edge-shared tetrahedral lattice. Both compounds show no magnetic order down to 0.35 K despite Curie-Weiss temperatures θCWθ_{CW} of -75.5 K (6H-B) and -182.5 K (3C), respectively. Below ∼25\sim 25 K the magnetic susceptibility of the 6H-B phase saturates to a constant value χ0=0.013χ_0 = 0.013 emu/mol which is followed below 7 K, by a linear-temperature dependent magnetic specific heat (CMC_M) displaying a giant coefficient γγ = 168 mJ/mol-K2^2. Both observations suggest the development of a Fermi-liquid like ground state characterized by a Wilson ratio of 5.6 in this insulating material. For the 3C phase, the CM∝T2C_M \propto T^2 behavior indicates a unique S=1, 3D QSL ground-state.

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