Ultrafast renormalization of the magnetic continuum in the proximal Kitaev quantum spin liquid H 3 LiIr 2 O 6 by tr-RIXS [Invited]
Jungho Kim, Tae‐Kyu Choi, Edward Mercer, Liam T. Schmidt, Jaeku Park, Sang‐Youn Park, Dogeun Jang, Seo Hyoung Chang, Ayman Said, Sae Hwan Chun, Kyeong Jun Lee, Sang Wook Lee, Hyunjeong Jeong, Hyeonhui Jeong, Chanhyeon Lee, Kwang‐Yong Choi, Faranak Bahrami, Fazel Tafti, Martin Claassen, A. de la Torre
We present the first circularly polarized non-resonant pump time-resolved resonant inelastic X-ray scattering (tr-RIXS) experiment in H 3 LiIr 2 O 6 , an iridium-based Kitaev system. Our calculations and experimental results are consistent with the modification of the low-energy magnetic excitations in H 3 LiIr 2 O 6 only during illumination by the laser pulse. We discuss these results in a cooperative framework between the Floquet engineering of the exchange interactions and the dynamic renormalization of electron-electron correlations. However, the penetration length mismatch between the X-ray probe and laser pump and the intrinsic complexity of Kitaev magnets prevents us from unequivocally extracting towards which ground state H 3 LiIr 2 O 6 is driven. We outline possible solutions to these challenges for light-driven stabilization and observation of the Kitaev quantum spin liquid limit by RIXS.
We present the first circularly polarized non-resonant pump time-resolved resonant inelastic X-ray scattering (tr-RIXS) experiment in H 3 LiIr 2 O 6 , an iridium-based Kitaev system. Our calculations and experimental results are consistent with the modification of the low-energy magnetic excitations in H 3 LiIr 2 O 6 only during illumination by the laser pulse. We discuss these results in a cooperative framework between the Floquet engineering of the exchange interactions and the dynamic renormalization of electron-electron correlations. However, the penetration length mismatch between the X-ray probe and laser pump and the intrinsic complexity of Kitaev magnets prevents us from unequivocally extracting towards which ground state H 3 LiIr 2 O 6 is driven. We outline possible solutions to these challenges for light-driven stabilization and observation of the Kitaev quantum spin liquid limit by RIXS.
We investigate the nonequilibrium dynamics of the transverse field Ising chain (TFIC) using time-resolved resonant inelastic X-ray scattering (tr-RIXS) in a pump-probe setup within a condensed matter setting. The tr-RIXS spectra reveal distinctive features, including two-kink continua at high energies and oscillatory spectral weight at low energies, both strongly influenced by the pump dynamics. By systematically analyzing the nonequilibrium tr-RIXS cross section under various pump configurations, we demonstrate how the spectra encode detailed information about the system's transient states, capturing instantaneous Hamiltonian parameters and the traversal of equilibrium quantum critical points during dynamic evolution. Notably, we uncover a one-to-one correspondence between oscillatory features in the low-energy spectra and dynamical quantum phase transitions, offering a novel and experimentally accessible approach for their detection. These findings highlight the versatility of tr-RIXS as a powerful tool for studying quantum systems far from equilibrium and their critical phenomena.
We calculate the resonant inelastic x-ray scattering (RIXS) response of the Kitaev honeycomb model, an exactly solvable quantum-spin-liquid model with fractionalized Majorana and flux excitations. We find that the fundamental RIXS channels, the spin-conserving (SC) and the non-spin-conserving (NSC) ones, do not interfere and give completely different responses. SC RIXS picks up exclusively the Majorana sector with a pronounced momentum dispersion, whereas NSC RIXS also creates immobile fluxes, thereby rendering the response only weakly momentum dependent, as in the spin structure factor measured by inelastic neutron scattering. RIXS can, therefore, pick up the fractionalized excitations of the Kitaev spin liquid separately, making it a sensitive probe to detect spin-liquid character in potential material incarnations of the Kitaev honeycomb model.
Motivated by the ongoing effort to search for high-resolution signatures of quantum spin liquids, we investigate the temperature dependence of the indirect resonant inelastic x-ray scattering (RIXS) response for the Kitaev honeycomb model. We find that, as a result of spin fractionalization, the RIXS response changes qualitatively at two well-separated temperature scales, TL and TH, which correspond to the characteristic energies of the two kinds of fractionalized excitations, Z2 gauge fluxes and Majorana fermions, respectively. While thermally excited Z2 gauge fluxes at temperature TL lead to a general broadening and softening of the response, the thermal proliferation of Majorana fermions at temperature ${T}_{H}\ensuremath{\sim}10\phantom{\rule{0.16em}{0ex}}{T}_{L}$ results in a significant shift of the spectral weight, both in terms of energy and momentum. Due to its exclusively indirect nature, the RIXS process we consider gives rise to a universal magnetic response and, from an experimental perspective, it directly corresponds to the K-edge of Ru3+ in the Kitaev candidate material $\ensuremath{\alpha}\ensuremath{-}{\mathrm{RuCl}}_{3}$.
We propose that resonant inelastic x-ray scattering (RIXS) is an effective probe of the fractionalized excitations in three-dimensional (3D) Kitaev spin liquids. While the non-spin-conserving RIXS responses are dominated by the gauge-flux excitations and reproduce the inelastic-neutron-scattering response, the spin-conserving (SC) RIXS response picks up the Majorana-fermion excitations and detects whether they are gapless at Weyl points, nodal lines, or Fermi surfaces. As a signature of symmetry fractionalization, the SC RIXS response is suppressed around the Γ point. On a technical level, we calculate the exact SC RIXS responses of the Kitaev models on the hyperhoneycomb, stripyhoneycomb, hyperhexagon, and hyperoctagon lattices, arguing that our main results also apply to generic 3D Kitaev spin liquids beyond these exactly solvable models.
Spin-orbit entangled materials have attracted widespread interest due to the novel magnetic phenomena arising from the interplay between spin-orbit coupling and electronic correlations. However, the intricate nature of spin interactions within Kiteav materials complicates the precise measurement of low-energy spin excitations. Using Na 2 Co 2 TeO 6 as an example, we study these low-energy spin excitations using the time-resolved resonant elastic x-ray scattering (tr-REXS). Our observations unveil remarkably slow spin dynamics at the magnetic peak, whose recovery timescale is several nanoseconds. This timescale aligns with the extrapolated spin gap of ~1 μ eV, obtained by density matrix renormalization group (DMRG) simulations in the thermodynamic limit. The consistency demonstrates the efficacy of tr-REXS in discerning low-energy spin gaps inaccessible to conventional spectroscopic techniques.
Abstract In recent years, there has been an intense search for materials realizing the Kitaev quantum spin liquid model. A number of edge-shared compounds with strong spin-orbit coupling, such as RuCl3 and iridates, have been proposed to realize this model. Nevertheless, an effective spin Hamiltonian derived from the microscopic model relevant to these compounds generally contains terms that are antagonistic toward the quantum spin liquid. This is consistent with the fact that the zero magnetic field ground state of these materials is generally magnetically ordered. It is a pressing issue to identify protocols to drive the system to the limit of the Kitaev quantum spin model. In this work, we propose Floquet engineering of these Kitaev quantum magnets by coupling materials to a circularly polarized laser. We demonstrate that all the magnetic interactions can be tuned in situ by the amplitude and frequency of the laser, hence providing a route to stabilize the Kitaev quantum spin liquid phase.