Many-Body Spin Correlations in Nonlinear Optical Spectroscopy

We study the role of spin correlations in nonlinear absorption due to optical transitions from a deep impurity level to states above a Fermi sea. We demonstrate that the Hubbard repulsion between two electrons occupying the impurity state leads to a logarithmic divergence of the third-order nonlinear optical susceptibility χ(3) at the absorption threshold. This divergence is a manifestation of the Kondo physics in the nonlinear optical response of Fermi sea systems. Remarkably, the light-induced Kondo temperature, which governs the shape of the Kondo-absorption spectrum, can be tuned by varying the intensity and frequency of the pump optical field. We also show that, for off-resonant pump excitation, the pump–probe spectrum exhibits a narrow peak below the linear absorption onset.