Perfect control of photoelectron anisotropy for randomly oriented ensembles of molecules by XUV REMPI and polarization shaping

Abstract

We report two schemes to generate perfect anisotropy in the photoelectron angular distribution of a randomly oriented ensemble of polyatomic molecules. In order to exert full control over the anisotropy of photoelectron emission, we exploit interferences between single-photon pathways and a manifold of resonantly-enhanced two-photon pathways. These are shown to outperform non-sequential $(\omega ,2\omega )$ bichromatic phase control for the example of CHFClBr molecules. We are able to optimize pulses that yield anisotropic photoelectron emission thanks to a very efficient calculation of photoelectron momentum distributions. This is accomplished by combining elements of quantum chemistry, variational scattering theory, and time-dependent perturbation theory.

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Cited by in corpus (6)

• Molecular chirality and its monitoring by ultrafast X-ray pulses
• Multi-photon above threshold ionization of multi-electron atoms and molecules using the R-matrix approach
• Disentangling enantiosensitivity from dichroism using bichromatic fields
• Numerical evaluation of orientation averages and its application to molecular physics
• Increasing ion yield circular dichroism in femtosecond photoionisation using optimal control theory
• General properties of the RABBITT at parity mixing conditions