We show that strongly photoexcited graphene monolayers with 35 fs pulses quasi-instantaneously build up a broadband, inverted Dirac fermion population. Optical gain emerges and directly manifests itself via a negative conductivity at the near-infrared region for the first 200 fs, where stimulated emission completely compensates absorption loss in the graphene layer. Our experiment-theory comparison with two distinct electron and hole chemical potentials reproduce absorption saturation and gain at 40 fs, revealing, particularly, the evolution of the transient state from a hot classical gas to a dense quantum fluid with increasing the photoexcitation.

The terahertz spectral regime, ranging from about 0.1-15 THz, is one of the least explored yet most technologically transformative spectral regions. One current challenge is to develop efficient and compact terahertz emitters/detectors with a broadband and gapless spectrum that can be tailored for various pump photon energies. Here we demonstrate efficient single-cycle broadband THz generation, ranging from about 0.1-4 THz, from a thin layer of split-ring resonators with few tens of nanometers thickness by pumping at the telecommunications wavelength of 1.5 mm (200 THz). The terahertz emission arises from exciting the magnetic-dipole resonance of the split-ring resonators and quickly decreases under off-resonance pumping. This, together with pump polarization dependence and power scaling of the terahertz emission, identifies the role of optically induced nonlinear currents in split-ring resonators. We also reveal a giant sheet nonlinear susceptibility B10 À 16 m 2 V À 1 that far exceeds thin films and bulk non-centrosymmetric materials.

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