High pressure sequence of Ba₃NiSb₂O₉ structural phases: new S = 1 quantum spin-liquids based on Ni²⁺

By using a high pressure, high temperature (HPHT) technique, the antiferromagnetically ordered ($T_N$ = 13.5 K) 6H-A phase of Ba$_3$NiSb$_2$O$_9$ was transformed into two new gapless quantum spin liquid(QSL) candidates with S=1 (Ni$^{2+}$) moments: the 6H-B phase with a Ni$^{2+}$-triangular lattice and the 3C-phase with a Ni$^{2+}$-three-dimensional (3D) edge-shared tetrahedral lattice. Both compounds show no magnetic order down to 0.35 K despite Curie-Weiss temperatures $\theta_{CW}$ of -75.5 K (6H-B) and -182.5 K (3C), respectively. Below $\sim 25$ K the magnetic susceptibility of the 6H-B phase saturates to a constant value $\chi_0 = 0.013 $ emu/mol which is followed below 7 K, by a linear-temperature dependent magnetic specific heat ($C_M$) displaying a giant coefficient $\gamma$ = 168 mJ/mol-K$^2$. 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 $C_M \propto T^2$ behavior indicates a unique S=1, 3D QSL ground-state.