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High harmonic generation in gases can be used as a probe of the electronic structure of the emitting medium, with attosecond temporal resolution and angström spatial resolution. The prospect of measuring molecular dynamics by pump-probe spectroscopy with such precision is attracting a lot of interest. An important issue in pump-probe spectroscopy lies in the ability to detect small signals: the detected signal can be easily dominated by the contributions from non-excited molecules or from a carrier gas. In this paper, we demonstrate that polarization-resolved pump-probe spectroscopy can be used to overcome this issue. We study high harmonic generation from rotationally excited molecules. We show that by measuring the harmonic field that is generated orthogonally to the driving laser field, the contrast in the detection of alignment revivals in nitrogen can be increased by a factor 4. We use this configuration to measure alignment revivals in an argon-nitrogen mixture, in which the total harmonic signal is dominated by the contributions from argon.

Polarization-resolved pump–probe spectroscopy with high harmonics