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

Autor: Loren Greenman, Christiane P. Koch, R. Esteban Goetz
Rok vydání: 2019
Předmět:
Zdroj: The Journal of Chemical Physics. 151:074106
ISSN: 1089-7690
0021-9606
DOI: 10.1063/1.5111362
Popis: 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.
Databáze: OpenAIRE