We report on the unusual behavior of the in-plane thermal conductivity κ and torque τ response in the Kitaev-Heisenberg material α-RuCl_{3}. κ shows a striking enhancement with linear growth beyond H=7  T, where magnetic order disappears, while τ for both of the in-plane symmetry directions shows an anomaly at the same field. The temperature and field dependence of κ are far more complex than conventional phonon and magnon contributions, and require us to invoke the presence of unconventional spin excitations whose properties are characteristic of a field-induced spin-liquid phase related to the enigmatic physics of the Kitaev model in an applied magnetic field.

Quantum spin systems such as magnetic insulators usually show magnetic order, but such classical states can give way to quantum liquids with exotic entanglement through two known mechanisms of frustration: geometric frustration in lattices with triangle motifs, and spin-orbit-coupling frustration in the exactly solvable quantum liquid of Kitaev’s honeycomb lattice. Here we present the experimental observation of a new kind of frustrated quantum liquid arising in an unlikely place: the magnetic insulator Ba4Ir3O10 where Ir3O12 trimers form an unfrustrated square lattice. The crystal structure shows no apparent spin chains. Experimentally we find a quantum liquid state persisting down to 0.2 K that is stabilized by strong antiferromagnetic interaction with Curie–Weiss temperature ranging from −766 to −169 K due to magnetic anisotropy. The anisotropy-averaged frustration parameter is 2000, seldom seen in iridates. Heat capacity and thermal conductivity are both linear at low temperatures, a familiar feature in metals but here in an insulator pointing to an exotic quantum liquid state; a mere 2% Sr substitution for Ba produces long-range order at 130 K and destroys the linear-T features. Although the Ir4+(5d5) ions in Ba4Ir3O10 appear to form Ir3O12 trimers of face-sharing IrO6 octahedra, we propose that intra-trimer exchange is reduced and the lattice recombines into an array of coupled 1D chains with additional spins. An extreme limit of decoupled 1D chains can explain most but not all of the striking experimental observations, indicating that the inter-chain coupling plays an important role in the frustration mechanism leading to this quantum liquid.

Insulating quantum magnets lie at the forefront both of fundamental research into quantum matter and of technological exploitation in the increasingly applied field of spintronics. In this context, the magnetic thermal transport is a particularly sensitive probe of the elementary spin and exotic topological excitations in unconventional magnetic materials. However, magnetic contributions to heat conduction are invariably intertwined with lattice (phonon) contributions, and thus the issue of spin-phonon coupling in determining the spin and thermal transport properties of magnetic insulators becomes more important with every emergent topological magnetic system. Here we report the observation of an anomalously strong enhancement of the thermal conductivity, occurring at all relevant temperatures, in the layered honeycomb material CrCl3 in the presence of an applied magnetic field. Away from the magnetically ordered phase at low temperatures and small fields, there is no coherent spin contribution to the thermal conductivity, and hence the effect must be caused by a strong suppression of the phonon thermal conductivity due to magnetic fluctations, which are in turn suppressed by the field. We build an empirical model for the thermal conductivity of CrCl3 within a formalism assuming an independently determined number of spin-flip processes and an efficiency of the phonon scattering events they mediate. By extracting the intrinsic phonon thermal conductivity we obtain a quantitative description of our measured data at all fields and temperatures, and we demonstrate that the scattering efficiency is entirely independent of the applied field. In this way we use CrCl3 as a model system to understand the interactions between spin and phonon excitations in the context of thermal transport. We anticipate that the completely general framework we introduce will have broad implications for the interpretation of transport phenomena in magnetic quantum materials.

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