Nature of Magnetic Excitations in the High-Field Phase of α-RuCl_{3}.

We present comprehensive electron spin resonance (ESR) studies of in-plane oriented single crystals of α-RuCl_{3}, a quasi-two-dimensional material with honeycomb structure, focusing on its high-field spin dynamics. The measurements were performed in magnetic fields up to 16 T, applied along the [110] and [100] directions. Several ESR modes were detected. Combining our findings with recent inelastic neutron- and Raman-scattering data, we identified most of the observed excitations. Most importantly, we show that the low-temperature ESR response beyond the boundary of the magnetically ordered region is dominated by single- and two-particle processes with magnons as elementary excitations. The peculiarities of the excitation spectrum in the vicinity of the critical field are discussed.

Destabilization of Magnetic Order in a Dilute Kitaev Spin Liquid Candidate.

The insulating honeycomb magnet α-RuCl_{3} exhibits fractionalized excitations that signal its proximity to a Kitaev quantum spin liquid state; however, at T=0, fragile long-range magnetic order arises from non-Kitaev terms in the Hamiltonian. Spin vacancies in the form of Ir^{3+} substituted for Ru are found to destabilize this long-range order. Neutron diffraction and bulk characterization of Ru_{1-x}Ir_{x}Cl_{3} show that the magnetic ordering temperature is suppressed with increasing x, and evidence of zizag magnetic order is absent for x>0.3. Inelastic neutron scattering demonstrates that the signature of fractionalized excitations is maintained over the full range of x investigated. The depleted lattice without magnetic order thus hosts a spin-liquid-like ground state that may indicate the relevance of Kitaev physics in the magnetically dilute limit of RuCl_{3}.

Antiferromagnetic Resonance and Terahertz Continuum in α-RuCl_{3}.

We report measurements of optical absorption in the zigzag antiferromagnet α-RuCl_{3} as a function of temperature T, magnetic field B, and photon energy ℏω in the range ∼0.3-8.3 meV, using time-domain terahertz spectroscopy. Polarized measurements show that threefold rotational symmetry is broken in the honeycomb plane from 2 to 300 K. We find a sharp absorption peak at 2.56 meV upon cooling below the Néel temperature of 7 K at B=0 that we identify as the magnetic-dipole excitation of a zero-wave-vector magnon, or antiferromagnetic resonance (AFMR). With the application of B, the AFMR broadens and shifts to a lower frequency as long-range magnetic order is lost in a manner consistent with transitioning to a spin-disordered phase. From a direct, internally calibrated measurement of the AFMR spectral weight, we place an upper bound on the contribution to the dc susceptibility from a magnetic excitation continuum.