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Abstract

We present polarization-controlled multiphoton two-color above-threshold ionization (TCATI) of molecules. The intensity modulations of valence photoelectron intensities of molecules arising from varying the relative orientation of the linear polarization vectors of femtosecond infrared (IR) and vacuum-ultraviolet (VUV) radiation in TCATI of the highest occupied molecular orbitals of $H_{2}O$, $O_{2}$, and $N_{2}$ are reported. The results on the molecular systems are compared to the $3p$ photoionization of atomic Ar, which serves as a reference system. Modeling the large differences of the modulation amplitudes within the soft-photon approximation enables us to extract the one-photon-ionization anisotropy parameter $β_{2}$. Accounting only for the first sideband due to two-photon TCATI by one VUV and one IR photon we find satisfactory agreement between experiment and simulation for $H_{2}O$ and $O_{2}$. However, the model fails for $N_{2}$ and possible reasons are discussed. We discuss that the described approach may represent an alternative way of determining photoelectron angular distributions from valence shells of molecules and indicate future directions for modeling TCATI of molecules.

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