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arXiv:2005.14189

Nonequilibrium quasistationary spin disordered state in the Kitaev-Heisenberg magnet $α$-RuCl$_3$

R. B. Versteeg, Alessio Chiocchetta, Fumiya Sekiguchi, A. I. R. Aldea, Anuja Sahasrabudhe, K. Budzinauskas, Zhe Wang, V. Tsurkan, Alois Loidl, Daniel I. Khomskii, Sebastian Diehl, Paul H. M. van Loosdrecht

Published May 28, 2020• 1 citation
arXivHTMLPDF

Abstract

Excitation by light pulses enables the manipulation of phases of quantum condensed matter. Here, we photoexcite high-energy holon-doublon pairs as a way to alter the magnetic free energy landscape of the Kitaev-Heisenberg magnet $α$-RuCl$_3$, with the aim to dynamically stabilize a proximate spin liquid phase. The holon-doublon pair recombination through multimagnon emission is tracked through the time-evolution of the magnetic linear dichroism originating from the competing zigzag spin ordered ground state. A small holon-doublon density suffices to reach a spin disordered state. The phase transition is described within a dynamic Ginzburg-Landau framework, corroborating the quasistationary nature of the transient spin disordered phase. Our work provides insight into the coupling between the electronic and magnetic degrees of freedom in $α$-RuCl$_3$ and suggests a new route to reach a proximate spin liquid phase in Kitaev-Heisenberg magnets.

DOI
10.48550/arxiv.2005.14189

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Nonequilibrium quasistationary spin disordered state in the Kitaev-Heisenberg magnet ααα-RuCl3_33​
Excitation by light pulses enables the manipulation of phases of quantum condensed matter. Here, we photoexcite high-energy holon-doublon pairs as a way to alter the magnetic free energy landscape of the Kitaev-Heisenberg magnet ααα-RuCl3_33​, with the aim to dynamically stabilize a proximate spin liquid phase. The holon-doublon pair recombination through multimagnon emission is tracked through the time-evolution of the magnetic linear dichroism originating from the competing zigzag spin ordered ground state. A small holon-doublon density suffices to reach a spin disordered state. The phase transition is described within a dynamic Ginzburg-Landau framework, corroborating the quasistationary nature of the transient spin disordered phase. Our work provides insight into the coupling between the electronic and magnetic degrees of freedom in ααα-RuCl3_33​ and suggests a new route to reach a proximate spin liquid phase in Kitaev-Heisenberg magnets.
We study the spin excitation spectra in magnetically ordered phases proximate to the Kitaev quantum spin liquid (KQSL). Although the low-energy universal features should be governed by the magnetic orders, the non-universal\textit{non-universal}non-universal high-energy features of the KQSL and adjacent phases can be remarkably similar. Therefore, we study the extended Kitaev model within a Stoner-like theory using Majorana partons, and compute the inelastic neutron scattering (INS) intensities in the random phase approximation. First, we benchmark against the antiferromagnetic (AFM) Heisenberg model and recover the AFM order with linear Goldstone modes. We then explore the phase diagram which agrees qualitatively with previous numerical results. In particular, the Majorana parton theory accurately captures Order-by-Disorder effects in the Kitaev-Heisenberg limit. We also find large INS intensities near the associated high-symmetry Brillouin zone (BZ) points of the magnetic orders. At intermediate and high energies, broad multi-spinon continua emerge across the BZ, providing a distinct mechanism for magnon decay and spectral broadening beyond the conventional multi-magnon decay scenario. Finally, we study the model Hamiltonian of candidate Kitaev material ααα-RuCl3_33​. The zigzag ground state agrees qualitatively with experiments, its stability under external magnetic field also exhibits strong anisotropy in the field directions, and broad scattering continua are recovered similar to those observed experimentally.
High-field fate of the Kitaev quantum spin liquid in ααα-RuCl3_33​
Kitaev quantum spin liquids (KQSLs) host fractionalized excitations described by itinerant Majorana quasiparticles and gapped Z2Z_2Z2​ fluxes (visons), providing a platform for emergent topological matter. Whether such a state survives under strong magnetic fields, however, remains an open question. The layered honeycomb magnet ααα-RuCl3_33​ is a leading candidate material: an in-plane field of ∼\sim∼ 7 T suppresses antiferromagnetic order and induces a quantum-disordered phase exhibiting signatures consistent with Majorana excitations, including an anomalous thermal Hall effect and field-angle-dependent specific heat. At higher fields, the magnetization approaches saturation, suggesting a transition to a spin-polarized state, yet the microscopic evolution between these limits remains unresolved. Here we report high-field specific heat measurements up to 24 T that reveal a distinct crossover at $μ_0H^*\approx$15 T, beyond which the perturbative Kitaev description breaks down. Above H∗H^*H∗, the characteristic six-fold angular modulation of the specific heat collapses and the excitation gap deviates from the predicted H3H^3H3 scaling. Meanwhile, the gap decreases with increasing field and the in-plane magnetization anisotropy persists up to ∼\sim∼ 24 T, both in sharp contrast to a trivial spin-polarized state, indicating that KQSL signatures are preserved even at ∼\sim∼ 90 % of magnetization saturation. These results reveal that the KQSL in ααα-RuCl3_33​ extends well beyond the perturbative window, persisting as a nonperturbative regime in which the Majorana and vison energy scales merge, before eventually giving way to spin polarization. This thermodynamic roadmap provides a basis for understanding how fractionalized phases evolve under strong magnetic fields.
Semiclassical Routes to the ααα-RuCl3_33​ Scattering Continuum via Model Meta−-−Analysis
ααα-RuCl3_33​ is a leading material for proximate Kitaev magnetism. We address the origin of the broad, ΓΓΓ-point centered excitation continuum observed by inelastic neutron scattering at elevated temperatures in this compound. Using stochastic Landau-Lifshitz dynamics augmented with quantum-equivalent corrections, we reproduce the temperature-dependent dynamical spin structure factor across both the correlated and conventional paramagnetic regimes. A meta-analysis of 38 published exchange parameter sets identifies those most consistent with the full temperature evolution. A Bayesian optimization procedure is used to derive parameters that capture the low-energy star-like momentum dependence and the overall bandwidth of the continuum. Rescaling temperatures by the Curie--Weiss scale produces a collapse of spectral measures, demonstrating that the high-TTT dynamics are governed by correlated paramagnetism below θCWθ_{\mathrm{CW}}θCW​ rather than by the Kitaev crossover to fractionalized excitations. Complementary 24-site exact diagonalization clarifies finite-size systematics at low temperature and the proximity to zigzag/incommensurate ordering. Beyond ααα-RuCl3_33​, our simulation pipeline provides a reproducible, data-driven framework to infer effective spin models in magnets that exhibit broad continua.
We introduce a matrix-product state based method to efficiently obtain dynamical response functions for two-dimensional microscopic Hamiltonians. We apply this method to different phases of the Kitaev-Heisenberg model and identify characteristic dynamical features. In the ordered phases proximate to the spin liquid, we find significant broad high-energy features beyond spin-wave theory, which resemble those of the Kitaev model. This establishes the concept of a proximate spin liquid, which was recently invoked in the context of inelastic neutron scattering experiments on α-RuCl_{3}. Our results provide an example of a natural path for proximate spin liquid features to arise at high energies above a conventionally ordered state, as the diffuse remnants of spin-wave bands intersect to yield a broad peak at the Brillouin zone center.
Detecting spin dynamics in quantum spin liquids presents significant challenges. Here, the authors explore photoinduced excitations in the Kitaev spin liquid candidate $\ensuremath{\alpha}$-RuCl3{}_{3}3​ using heterodyne transient grating spectroscopy. This method allows for a comprehensive characterization of different photoinduced components. They identify signatures of spin excitations within the Kitaev paramagnetic phase. The two distinct lifetimes observed in this temperature regime, on the order of tens of picoseconds, likely correspond to the dynamics of unconventional spin excitations predicted by the Kitaev model.
Raman and terahertz spectroscopy, combined with exact diagonalization studies, reveal the nature of the high-field phase of the proximate Kitaev material $\ensuremath{\alpha}$-RuCl3{}_{3}3​ as a partially polarized quantum disordered state. The state is characterized by a gapped multiparticle continuum, out of which a two-particle bound state emerges, together with a well-defined single-particle excitation at low energy. The results underline the unusual nature of the high-field phase, and the important role of Kitaev and off-diagonal interactions in $\ensuremath{\alpha}$-RuCl3{}_{3}3​.