Cascaded four-wave mixing in the XUV region.

We present a detailed study of the wave-mixing process in the extreme ultraviolet (XUV) region (around 30 nm) by using two collinear multiple-cycle laser pulses with incommensurate frequencies (wavelengths 1400 and 800 nm). The experimental data provide evidence for the coherent accumulation of wave-mixing fields and a high third-order response of the medium in this spectral range. We show that the time evolution of the mixing fields can be used to study the coherence dynamics of the free-electron wave packet with a lifetime of 200-750 fs.

Spectrally resolved femtosecond two-color three-pulse photon echoes: study of ground and excited state dynamics in molecules.

We report the use of spectrally resolved femtosecond two-color three-pulse photon echoes as a potentially powerful multidimensional technique for studying vibrational and electronic dynamics in complex molecules. The wavelengths of the pump and probe laser pulses are found to have a dramatic effect on the spectrum of the photon echo signal and can be chosen to select different sets of energy levels in the vibrational manifold, allowing a study of the dynamics and vibrational splitting in either the ground or the excited state. The technique is applied to studies of the dynamics of vibrational electronic states in the dye molecule Rhodamine 101 in methanol.