Unambiguous identification of fractionalized excitations in quantum spin liquids has been a long-standing issue in correlated topological phases. Conventional spectroscopic probes, such as the dynamical spin structure factor, can only detect composites of fractionalized excitations, leading to a broad continuum in energy. Lacking a clear signature in conventional probes has been the biggest obstacle in the field. In this work, we theoretically investigate what kinds of distinctive signatures of fractionalized excitations can be probed in two-dimensional nonlinear spectroscopy by considering the exactly solvable Kitaev spin liquids. We demonstrate the existence of a number of salient features of the Majorana fermions and fluxes in two-dimensional nonlinear spectroscopy, which provide crucial information about such excitations.

• Received 3 December 2019
• Accepted 28 February 2020

DOI:https://doi.org/10.1103/PhysRevLett.124.117205