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

Abstract

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.

4 pages, 3 figures

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