Population inversion and ultrafast terahertz nonlinearity of transient Dirac fermions in Cd₃As₂

Harmonic generation provides an efficient tool for the study of ultrafast nonlinear dynamics. We report on time-resolved optical-pump terahertz-harmonic-generation spectroscopic investigation of ultrafast nonlinearity in a prototypical three-dimensional Dirac semimetal Cd$_3$As$_2$. A transient population inversion characterized by excessive nonthermal Dirac electrons and holes is found to be very sensitive and responsive to a periodic terahertz drive, leading to very efficient terahertz third-harmonic generation. Based on the Boltzmann transport theory, we analyze the terahertz field-driven kinetics of the transient Dirac fermions that is responsible for the observed strong terahertz nonlinearity.