We propose a method, molecular polarimetry, applicable to an extended VUV-x-ray range, allowing us to determine the complete state of elliptically polarized light, including the challenging disentanglement of the circular and unpolarized components. It relies on the determination of the molecular frame photoelectron angular distributions derived from electron-ion velocity vector correlations in dissociative photoionization of simple molecules. The high accuracy of the full set of Stokes parameters determination has been established by comparison with data obtained in parallel with a VUV optical polarimeter used as a benchmark.
High harmonics generated by counter-rotating laser fields at the fundamental and second harmonic frequencies have raised important interest as a table-top source of circularly polarized ultrashort extreme-ultraviolet light. However, this emission has not yet been fully characterized: in particular it was assumed to be fully polarized, leading to an uncertainty on the effective harmonic ellipticity. Here we show, through simulations, that ultrashort driving fields and ultrafast medium ionization lead to a breaking of the dynamical symmetry of the interaction, and consequently to deviations from perfectly circular and fully polarized harmonics, already at the single-atom level. We perform the complete experimental characterization of the polarization state of high harmonics generated along that scheme, giving direct access to the ellipticity absolute value and sign, as well as the degree of polarization of individual harmonic orders. This study allows defining optimal generation conditions of fully circularly polarized harmonics for advanced studies of ultrafast dichroisms.
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