Abstract

It is shown that by measuring the angular distributions of fragmented ions of simple molecules by sub-10 fs laser pulses at intensities in the non-sequential double ionization regime the electron density of the highest occupied molecular orbital can be probed directly. For pulses of a few tens of femtoseconds or longer, it is shown that the angular distributions of the ions are dominated by post-ionization alignment which results from the additional rotation of the molecular axis during the breakup process. These models are used to explain recent experiments.

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