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

• URL: http://arxiv.org/abs/2202.12235v1
• Date: Fri, 18 Feb 2022 12:00:25 GMT
• Title: Increasing ion yield circular dichroism in femtosecond photoionisation using optimal control theory
• Authors: Manel Mondelo-Martell (1) and Daniel Basilewitsch (1) and Hendrike Braun (2) and Christiane P. Koch (1) and Daniel M. Reich (1) ((1) Dahlem Center of Complex Quantum Systems & Department of Physics, Freie Universit\"at Berlin, Berlin. (2) Institute of Physics, Universit\"at Kassel, Kassel)
• Abstract summary: We find that the absolute CD signal of randomly oriented molecules can be increased by a factor 3.5 when using shaped laser pulses. Our insights provide additional evidence on how optimal control can assist in amplifying chiral signatures.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: We investigate how optimal control theory can be used to improve Circular Dichroism (CD) signals for 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 (~8%) but also 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 3.5 when using shaped laser pulses, with the anisotropy parameter g increasing from 0.06 to 1. Our insights provide additional evidence on how optimal control can assist in amplifying chiral signatures via interactions of permanent and transition multipole moments.

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