We report time-resolved optical pump-terahertz third-harmonic generation spectroscopy of picosecond nonthermal many-body charge dynamics in high-purity silicon at room temperature. Although in thermal equilibrium excitons in silicon are unstable due to a lower binding energy than the thermal energy at room temperature, following pulsed nonresonant optical pumping we can identify the formation of transient excitonic states on the picosecond timescale in our high-resolution nonlinear spectroscopic measurements. In contrast to unbound electron-hole pairs, the nonthermal many-body excitonic dynamics feature a characteristic time-dependent evolution, a distinct dependence on charge density, and a nonperturbative nonlinear terahertz response.

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• Excitons
• Quantum many-body systems
• Semiconductors
• High-harmonic generation
• Terahertz spectroscopy