Spin-orbital liquid state assisted by singlet-triplet excitation in $J=0$ ground state of Ba${}_3$ZnIr${}_2$O${}_9$

Abstract

Strong spin-orbit coupling (SOC) effects of heavy $d$-orbital elements have long been neglected in describing the ground states of their compounds thereby overlooking a variety of fascinating and yet unexplored magnetic and electronic states, until recently. The spin-orbit entangled electrons in such compounds can get stabilized into unusual spin-orbit multiplet $J$-states which warrants severe investigations. Here we show using detailed magnetic and thermodynamic studies and theoretical calculations the ground state of Ba${}_3$ZnIr${}_2$O${}_9$, a 6$H$ hexagonal perovskite is a close realisation of the elusive $J$~=~0 state. However, we find that local Ir moments are spontaneously generated due to the comparable energy scales of the singlet-triplet splitting driven by SOC and the superexchange interaction mediated by strong intra-dimer hopping. While the Ir ions within the structural Ir${}_2$O${}_9$ dimer prefers to form a spin-orbit singlet state (SOS) with no resultant moment, substantial interdimer exchange interactions from a frustrated lattice ensure quantum fluctuations till the lowest measured temperatures and stabilize a spin-orbital liquid phase.

Main Text: 6 pages, 4 figures, 1 table; Supplementary: 4 pages, 2 figures, 2 tables

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