We study high-order harmonic generation in aligned molecules close to the ionization threshold. Two distinct contributions to the harmonic signal are observed, which show very different responses to molecular alignment and ellipticity of the driving field. We perform a classical electron trajectory analysis, taking into account the significant influence of the Coulomb potential on the strong-field-driven electron dynamics. The two contributions are related to primary ionization and excitation processes, offering a deeper understanding of the origin of high harmonics near the ionization threshold. This Letter shows that high-harmonic spectroscopy can be extended to the near-threshold spectral range, which is in general spectroscopically rich.

We demonstrate that the synchronization effect observed [Pedersen et al., Phys. Rev. Lett. 87, 055001 (2001)]], when a bunch of ions oscillates between two mirrors in an electrostatic ion beam trap, can be explained as a negative mass instability. We derive simple necessary conditions for the existence of a regime in which this dispersionless behavior occurs and demonstrate that in this regime, the ion trap can be used as a high resolution mass spectrometer.

The temporal evolution of the dissociation probabilities for various vibrational levels of H 2 + is observed in terms of shifts in the kinetic energy release dissociation spectra, induced by linearly chirped intense laser pulses. In contrast to previous observations, in which no dependence on the chirp sign was observed, the energy spectrum reported here shows peak shifts, up for negative chirp and down for positive chirp. For some vibrational levels, dissociation takes place early on in the pulse; hence, care must be taken while interpreting the effect of pulse duration in photodissociation studies. This interpretation is supported by numerical solutions of the time-dependent Schrödinger equation.

We describe a system combining an ion beam trap and a low energy electron target in which the interaction between electrons and vibrationally cold molecular ions and clusters can be studied. The entire system uses only electrostatic fields for both trapping and focusing, thus being able to store particles without a mass limit. Preliminary results for the electron impact neutralization of C 2 − ions and aluminum clusters are presented.

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