Origin of strong-field-induced low-order harmonic generation in amorphous quartz

Abstract

Kerr-type nonlinearities form the basis for our physical understanding of nonlinear optical phenomena in condensed matter, such as self-focusing, solitary waves and wave mixing1–3. In strong fields, they are complemented by higher-order nonlinearities that enable high-harmonic generation, which is currently understood as the interplay of light-driven intraband charge dynamics and interband recombination4–6. Remarkably, the nonlinear response emerging from the subcycle injection dynamics of electrons into the conduction band, that is from ionization, has been almost completely overlooked in solids and only partially considered in the gas phase7–10. Here, we reveal this strong-field-induced nonlinearity in a-SiO2 as a typical wide-bandgap dielectric by means of time-resolved, low-order wave-mixing experiments, and show that, close to the material damage threshold, the so far unexplored injection current provides the leading contribution. The sensitivity of the harmonic emission to the subcycle ionization dynamics offers an original approach to characterize the evolution of laser-induced plasma formation in optical microprocessing. Strong-field-induced nonlinearities from the injection of electrons into the conduction band contribute to harmonic generation in amorphous quartz. Close to the damage threshold, they dominate over intraband and interband contributions.