Exploring Two-dimensional Coherent Spectroscopy with Exact Diagonalization: Spinons and Confinement in 1D Quantum Magnets

Two-dimensional coherent spectroscopy (2DCS) with terahertz radiation offers a promising new avenue for the exploration of many-body phenomena in quantum magnets. This includes the potential diagnosis of fractionalized excitations, for which linear response often struggles due to the indistinguishability of a continuum of fractional excitations from that caused by disorders or impurities. However, the interpretation of the complex results produced by 2DCS remains a challenge, and a general prediction of the spectral characteristics of different types of excitations has not yet been established. In this paper, we develop a numerical approach based on exact diagonalization (ED) to push our understanding of 2DCS towards different scenarios. We first validate our approach by comparing numerical ED and exact analytical results for the spectroscopic signatures of spinons in one-dimensional transverse field Ising model and develop how to deal with the inherently small system sizes in ED calculations. Augmenting the model by a longitudinal field, we demonstrate significant changes to the 2DCS spectrum upon the field-induced spinon pair confinement, which can be rationalized in our ED calculations and from a "two-kink" model (in the absence of integrability). One advantage of our ED approach is its possible extension to finite temperatures, which we explore using thermally pure quantum states and demonstrate to change the intensity and spectroscopical patterns of 2DCS when going beyond the integrable model. Our numerically exact results provide a benchmark for future experiments and theoretical studies relying on approximation methods, and pave the way for the exploration of fractionalized excitations in quantum magnets.