Two-dimensional coherent spectroscopy of CoNb$_2$O$_6$

Abstract

With recent advances in terahertz (THz) sources and detection, two-dimensional coherent spectroscopy (2DCS), which allows to probe nonlinear responses in a two-frequency plane, now reaches the meV regime relevant for quasiparticle excitations in magnetic materials. This opens a promising route to reveal many-body phenomena that evade linear-response probes. To date most experimental applications have focused on classical magnets, and a solid demonstration in a quantum magnet has yet to be established. Here we present a theoretical study of 2DCS in CoNb$_2$O$_6$, a quasi-one-dimensional Ising magnet that is believed to host fractionalized spinons which at low temperatures are confined by weak interchain coupling. Our analysis, which builds on an effective $S=1/2$ Hamiltonian is found to reveal unambiguous 2DCS signatures of spinon deconfinement above the low-temperature ordered phase. Using a four-spinon approximation, we track these 2DCS signatures by sequentially building a faithful microscopic model for CoNb$_2$O$_6$, starting from the exactly solvable one-dimensional transverse-field Ising model (1$d$ TFIM) and successively adding interactions to capture its key low-energy physics. In particular, adding a bond-dependent staggered YZ interaction to the 1$d$-TFIM already reproduces many key spectral features of the full material Hamiltonian. Within this TFIM+YZ model, we find a series of bound states, including a four-spinon bound state that is distinct from the familiar two-spinon bound states. We further find that introducing a confinement potential suppresses sharp spinon-echo features in the two-frequency space, which are thought to reflect an underlying continuum of fractionalized excitations. Our results provide concrete predictions and clear targets for future THz 2DCS experiments on CoNb$_2$O$_6$ and related quasi-one-dimensional quantum magnets.