High-contrast pump-probe spectroscopy with high-order harmonics

Abstract : The high order harmonic generation process from molecules can be used to probe the structure of the emitting medium with high spatial resolution[1,2]. The measurements of molecular dynamics with such a probe is thus very appealing. Contrast is an important issue in pump probe spectroscopy: in general the probe only excites part of the molecules, so that the detected signal can be dominated by contributions from non-excited molecules. In this article we review two techniques that can be used to enhance the contrast of pump probe measurements: transient grating spectroscopy and polarization-resolved spectroscopy. We use these techniques to detect rotational wavepackets and demonstrate a dramatic improvement in the contrast of the measured signal.
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Y Mairesse, W Boutu, P Breger, E Constant, D Descamps, et al.. High-contrast pump-probe spectroscopy with high-order harmonics. France. EDP Sciences, pp.107-111, 2009, UVX 2008, ⟨10.1051/uvx/2009017⟩. ⟨hal-01164784⟩

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