Disentangling spin excitation continua in classical and quantum magnets using two-dimensional nonlinear spectroscopy

Inelastic neutron scattering (INS) has traditionally been one of the primary methods for investigating quantum magnets, particularly in identifying a continuum of excitations as a hallmark of spin fractionalization in quantum spin liquids (QSLs). However, INS faces severe limitations due to its inability to distinguish between such QSL signatures and similar excitation continua arising from highly frustrated magnetic orders with large unit cells or classical spin liquids. In contrast, two-dimensional coherent spectroscopy (2DCS) has emerged as a powerful tool to probe nonlinear excitation dynamics, offering insights into the underlying mechanisms behind these broad spectral features. In this paper, we utilize classical molecular dynamics techniques to explore the 2DCS responses of frustrated magnets with dominant Kitaev interactions. Comparing the classical and quantum versions of the pure Kitaev model, our results indicate both clear similarities, in the form of sharp line features, and clear distinctions, in the locations of these features and in selection rules. Moreover, in the extended 𝐾⁢Γ⁢Γ′ model, we show that the 2DCS response of the Kitaev spin liquid is completely distinct from that of large unit cell magnetic orders, despite both generating a broad continuum in INS. Additionally, we demonstrate the extreme sensitivity of classical 2DCS to thermal fluctuations and discuss the potential significance of quantum coherence in experimental settings. Overall, our paper illustrates the potential of 2DCS in resolving the complex physics underlying ambiguous spin excitation continua, thereby enhancing our understanding of the dynamics in these frustrated systems.