Issue 16, 2022

Increasing ion yield circular dichroism in femtosecond photoionisation using optimal control theory

Abstract

We investigate how optimal control theory can be used to improve Circular Dichroism (CD) signals for the A-band of fenchone measured via the photoionization yield upon further excitation. These transitions are electric dipole forbidden to first order, which translates into low population transfer to the excited state but allows for a clearer interplay between electric and magnetic transition dipole moments, which are of the same order of magnitude. Using a model including the electronic ground and excited A state as well as all permanent and transition multipole moments up to the electric quadrupole, we find that the absolute CD signal of randomly oriented molecules can be increased by a factor of 2.5 when using shaped laser pulses, with the anisotropy parameter g increasing from 0.06 to 1. We find that this effect is caused by the interference between the excitation pathways prompted by the different multipole moments of the molecule.

Graphical abstract: Increasing ion yield circular dichroism in femtosecond photoionisation using optimal control theory

Associated articles

Article information

Article type
Paper
Submitted
15 11 2021
Accepted
17 2 2022
First published
12 4 2022
This article is Open Access
Creative Commons BY-NC license

Phys. Chem. Chem. Phys., 2022,24, 9286-9297

Increasing ion yield circular dichroism in femtosecond photoionisation using optimal control theory

M. Mondelo-Martell, D. Basilewitsch, H. Braun, C. P. Koch and D. M. Reich, Phys. Chem. Chem. Phys., 2022, 24, 9286 DOI: 10.1039/D1CP05239J

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