Nonlinear light conversion involves one or more bound–bound, bound–free, free–free, and free–bound transitions. It is often challenging to interpret the exact conversion mechanisms. Here we use a femtosecond mid-infrared laser to enhance free–free transitions in terahertz and Brunel harmonic generation from air plasma. Microscopically, both THz and harmonics originate from a common source–ionization-induced plasma currents–and are greatly enhanced when driven by intense long-wavelength pulses. We observe 1% laser-to-terahertz conversion efficiency. Using two-color laser fields, we generate coherent radiation from terahertz to petahertz and investigate the interplay among tunneling ionization, terahertz, and harmonic generation with coherent control.
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