Quantum magnetism and quantum phase transitions

Abstract:

Kitaev materials often order magnetically at low temperatures due to the presence of non-Kitaev interactions. Torque magnetometry is a very sensitive technique for probing the magnetic anisotropy, which is critical in understanding the magnetic ground state. In this work, we report detailed single-crystal torque measurements in the proposed Kitaev candidate honeycomb magnet α-RuBr3, which displays zigzag order below 34 K. Based on angular-dependent torque studies in magnetic fields up to 16 T rotated in the plane normal to the honeycomb layers, we find an easy-plane anisotropy with a temperature dependence of the torque amplitude following closely the behaviour of the powder magnetic susceptibility. The torque for field rotated in the honeycomb plane has a clear six-fold periodicity with a saw-tooth shape, reflecting the three-fold symmetry of the crystal structure and stabilization of different zigzag domains depending on the field orientation, with a torque amplitude that follows an order parameter form inside the zigzag phase. By comparing experimental data with theoretical calculations we highlight the importance of relevant anisotropic interactions and the role of the competition between different zigzag domains in this candidate Kitaev magnet.

Abstract:

The physics of spin-orbit entangled magnetic moments of 4d and 5d transition metal ions on a honeycomb lattice has been much explored in the search for unconventional magnetic orders or quantum spin liquids expected for compass spin models, where different bonds in the lattice favour different orientations for the magnetic moments. Realising such physics with rare-earth ions is a promising route to achieve exotic ground states in the extreme spin-orbit limit; however, this regime has remained experimentally largely unexplored due to major challenges in materials synthesis. Here we report the successful synthesis of powders and single crystals of β-Na₂PrO₃, with 4f¹ Pr⁴⁺ j_eff = 1/2 magnetic moments arranged on a hyperhoneycomb lattice with the same threefold coordination as the planar honeycomb. We find a strongly non-collinear magnetic order with highly dispersive gapped excitations that we argue arise from frustration between bond-dependent, anisotropic off-diagonal exchanges, a compass quantum spin model not explored experimentally so far. Our results show that rare-earth ions on threefold coordinated lattices offer a platform for the exploration of quantum compass spin models in the extreme spin-orbit regime, with qualitatively distinct physics from that of 4d and 5d Kitaev materials.

Abstract:

In the Kitaev honeycomb model, spins coupled by strongly-frustrated anisotropic interactions do not order at low temperature but instead form a quantum spin liquid with spin fractionalisation into Majorana fermions and static fluxes. The realization of such a model in crystalline materials could lead to major breakthroughs in understanding entangled quantum states, however achieving this in practice is a very challenging task. The recently synthesized honeycomb material RuI3 shows no long-range magnetic order down to the lowest probed temperatures and has been theoretically proposed as a quantum spin liquid candidate material on the verge of an insulator to metal transition. Here we report a comprehensive study of the magnetic anisotropy in un-twinned single crystals via torque magnetometry and detect clear signatures of strongly anisotropic and frustrated magnetic interactions. We attribute the development of sawtooth and six-fold torque signal to strongly anisotropic, bond-dependent magnetic interactions by comparing to theoretical calculations. As a function of magnetic field strength at low temperatures, torque shows an unusual non-parabolic dependence suggestive of a proximity to a field-induced transition. Thus, RuI3, without signatures of long-range magnetic order, displays key hallmarks of an exciting candidate for extended Kitaev magnetism with enhanced quantum fluctuations.