Abstract

We report a modulation of third-harmonic generation (THG) owing to a rotational coherence in ${\mathrm{CO}}_2$. The variation in conversion efficiency is mostly attributed to the dependence of ${\chi }^{\left(3\right)}\left(\tau \right)$ on the molecular alignment. THG via type I processes mainly depends on ${\chi }^{\left(3\right)}\left(\tau \right)$, while type II processes are influenced by the wave packet owing to both ${\chi }^{\left(3\right)}\left(\tau \right)$ and $\mathrm{\Delta }k\left(\tau \right)$. Observation of the generated third harmonic also shows significant changes of the polarization state owing to the birefringence induced by the rotational wave packet. Numerical modeling shows good qualitative agreement with the experimental data.

© 2008 Optical Society of America

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