Strong terahertz third-harmonic generation by kinetic heavy quasiparticles in CaRuO₃

We report on time-resolved nonlinear terahertz spectroscopy of a strongly correlated ruthenate, CaRuO$_3$, as a function of temperature, frequency and terahertz field strength. Third-harmonic radiation for frequencies up to 2.1 THz is observed evidently at low temperatures below 80 K, where the low-frequency linear dynamical response deviates from the Drude model and a coherent heavy quasiparticle band emerges by strong correlations associated with the Hund's coupling.Phenomenologically, by taking an experimentally observed frequency-dependent scattering rate, the deviation of the field driven kinetics from the Drude behavior is reconciled in a time-dependent Boltzmann description, which allows an attribution of the observed third-harmonic generation to the terahertz field driven nonlinear kinetics of the heavy quasiparticles.