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

## TL;DR

This paper introduces two innovative schemes to achieve perfect control over photoelectron anisotropy in randomly oriented polyatomic molecules using XUV REMPI and polarization shaping, surpassing previous bichromatic phase control methods.

## Contribution

The authors develop and demonstrate two schemes leveraging interference of photon pathways for complete anisotropy control, integrating quantum chemistry, scattering theory, and perturbation theory.

## Key findings

- Achieved perfect anisotropy in photoelectron emission.
- Outperformed traditional bichromatic phase control.
- Optimized pulses for anisotropic emission.

## 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.