Perfect control of photoelectron anisotropy for randomly oriented ensembles of molecules by XUV REMPI and polarization shaping
R. Esteban Goetz, Christiane P. Koch, Loren Greenman
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.
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 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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