We report a new classical spin liquid in which the collective flux degrees of freedom break the translation symmetry of the honeycomb lattice. This exotic phase exists in frustrated spin-orbit magnets where a dominant off-diagonal exchange, the so-called Γ term, results in a macroscopic ground-state degeneracy at the classical level. We demonstrate that the system undergoes a phase transition driven by thermal order-by-disorder at a critical temperature Tc ≈ 0.04|Γ|. At first sight, this transition reduces an emergent spherical spin-symmetry to a cubic one: spins point predominantly toward the cubic axes at T < Tc. However, this seems to simply restore the cubic symmetry of the Γ model, and the non-coplanar spins remain disordered below Tc. We show that the phase transition actually corresponds to plaquette ordering of hexagonal fluxes and the cubic symmetry is indeed broken, a scenario that is further confirmed by our extensive Monte Carlo simulations.
The leading order nonlinear (NL) susceptibility, χ3, in a paramagnet is negative and diverges as T → 0. This divergence is destroyed when spins correlate and the NL response provides unique insights into magnetic order. Dimensionality, exchange interaction, and preponderance of quantum effects all imprint their signatures in the NL magnetic response. Here, we study the NL susceptibilities in the proximate Kitaev magnet α-RuCl3, which differs from the expected antiferromagnetic behavior. For T < Tc = 7.5 K and field B in the ab-plane, we obtain contrasting NL responses in low (<2 T) and high field regions. For low fields, the NL behavior is dominated by a quadratic response (positive χ2), which shows a rapid rise below Tc. This large χ2 > 0 implies a broken sublattice symmetry of magnetic order at low temperatures. Classical Monte Carlo (CMC) simulations in the standard K − H − Γ model secure such a quadratic B dependence of M, only for T ≈ Tc with χ2 being zero as T → 0. It is also zero for all temperatures in exact diagonalization calculations. On the other hand, we find an exclusive cubic term (χ3) that describes the high field NL behavior well. χ3 is large and positive both below and above Tc crossing zero only for T > 50 K. In contrast, for B ∥ c-axis, no separate low/high field behaviors are measured and only a much smaller χ3 is apparent.
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