Single-cycle terahertz (THz) transients in the frequency range 0.3-7 THz with electric-field amplitudes of more than 400 kV/cm are generated by four-wave mixing of the fundamental and the second harmonic of 25 fs pulses from a Ti:sapphire amplifier in ionized air. These transients are fully characterized by electro-optic sampling with ZnTe and GaP crystals. One can tune the center frequency of the THz transients by varying the length of the incident pulse. The electric-field amplitude increases linearly with the incident pulse energy.

Reversible structural changes of a nanostructure were measured nondestructively with subpicometer spatial and subpicosecond temporal resolution via x-ray diffraction (XRD). The spatially periodic femtosecond excitation of a gallium arsenide/aluminum gallium arsenide superlattice results in coherent lattice motions with a 3.5-picosecond period, which was directly monitored by femtosecond x-ray pulses at a 1-kilohertz repetition rate. Small changes (DeltaR/R = 0.01) of weak Bragg reflexes (R = 0.005) were detected. The phase and amplitude of the oscillatory XRD signal around a new equilibrium demonstrate that displacive excitation of the zone-folded acoustic phonons is the dominant mechanism for strong excitation.

We present a combined theoretical and experimental study of spatiotemporal propagation effects in terahertz (THz) generation in gases using two-color ionizing laser pulses. The observed strong broadening of the THz spectra with increasing gas pressure reveals the prominent role of spatiotemporal reshaping and of a plasma-induced blueshift of the pump pulses in the generation process. Results obtained from (3+1)-dimensional simulations are in good agreement with experimental findings and clarify the mechanisms responsible for THz emission.

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