When an intense laser pulse is focused into a gas, the light-atom interaction that occurs as atoms are ionized results in an extremely nonlinear optical process--the generation of high harmonics of the driving laser frequency. Harmonics that extend up to orders of about 300 have been reported, some corresponding to photon energies in excess of 500 eV. Because this technique is simple to implement and generates coherent, laser-like, soft X-ray beams, it is currently being developed for applications in science and technology; these include probing the dynamics in chemical and materials systems and imaging. Here we report that by carefully tailoring the shapes of intense light pulses, we can control the interaction of light with an atom during ionization, improving the efficiency of X-ray generation by an order of magnitude. We demonstrate that it is possible to tune the spectral characteristics of the emitted radiation, and to steer the interaction between different orders of nonlinear processes.

Cross-correlation frequency-resolved optical gating with an angle-dithered nonlinear-optical crystal permits measurement of the intensity and the phase of the ultrabroadband (as much as 1200 nm wide) continuum generated from microstructure optical fiber. Retrieval revealed fine-scale structure in the continuum spectrum. Simulations and single-shot spectrum measurements confirmed that the fine structure does exist on a single-shot basis but washes out when many shots are averaged.

An electrostatically deformable, gold-coated, silicon nitride membrane mirror was used as a phase modulator to compress pulses from 92 to 15 fs. Both an iterative genetic algorithm and single-step dispersion compensation based on frequency-resolved optical gating calibration of the mirror were used to compress pulses to within 10% of the transform limit. Frequency-resolved optical gating was used to characterize the pulses and to test the range of the deformable-mirror-based compressor.

Pulse-front tilt in an ultrashort laser pulse is generally considered to be a direct consequence of, and equivalent to, angular dispersion. We show, however, that, while this is true for certain types of pulse fields, simultaneous temporal chirp and spatial chirp also yield pulse-front tilt, even in the absence of angular dispersion. We verify this effect experimentally using GRENOUILLE.