International audienceCircular dichroism in the extreme ultraviolet range is broadly used as a sensitive structural probe of matter, from the molecular photoionization of chiral species1, 2, 3 to the magnetic properties of solids4. Extending such techniques to the dynamical regime has been a long-standing quest of solid-state physics and physical chemistry, and was only achieved very recently5 thanks to the development of femtosecond circular extreme ultraviolet sources. Only a few large facilities, such as femtosliced synchrotrons6, 7 or free-electron lasers8, are currently able to produce such pulses. Here, we propose a new compact and accessible alternative solution: resonant high-order harmonic generation of an elliptical laser pulse. We show that this process, based on a simple optical set-up, delivers bright, coherent, ultrashort, quasi-circular pulses in the extreme ultraviolet. We use this source to measure photoelectron circular dichroism on chiral molecules, opening the route to table-top time-resolved femtosecond and attosecond chiroptical experiments

High-order harmonic generation in polyatomic molecules generally involves multiple channels of ionization. Their relative contribution can be strongly influenced by the presence of resonances, whose assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach for the investigation of unaligned polyatomic molecules, using SF6 as an example. We combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Fragment-resolved above-threshold ionization measurements reveal that strong-field ionization opens at least three channels. A shape resonance in one of them is found to dominate the signal in the 20–26 eV range. This resonance induces a phase jump in the harmonic emission, a switch in the polarization state and different dynamical responses to molecular vibrations. This study demonstrates a method for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected.