Abstract
High-order harmonic emission from aligned molecules can be used as a probe of molecular structure with ultrafast time resolution. In this paper, we review past work, and also present new measurements of the intensity and phase of harmonic emission from N 2O and N 2 molecules. We find that high harmonic emission from CO 2 and N 2O molecules is well described by a simple two-center interference model. In contrast, high harmonic emission from N 2 exhibits a very different behavior, not readily explained by assuming that the electron responsible for the high-order harmonic emission recollides with the molecule as a plane wave. These data clearly emphasize the need for more comprehensive models of high harmonic generation from molecules.
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