ORCID
https://orcid.org/0000-0003-2849-9379
Date of Award
9-7-2023
Degree Name
Doctor of Philosophy (PhD)
Degree Type
Dissertation
Abstract
Comparing experimental photoelectron angular distributions to theoretical predictions for direct detachment is a valuable tool for indicating more complex detachment pathways, such as those which access temporary anion states. This is exemplified by resonance mediated detachment from NiO2−. The presence of forbidden transitions and deviations in photoelectron angular distribution and relative transition intensities indicate a resonance, which is further supported with multireference calculations. In detachment processes that produce a neutral molecule with a permanent dipole, the quality of angular distribution predictions suffer by treating the outgoing electron as a free particle. To improve upon this issue, angular distribution prediction methods are developed to incorporate the effect of the charge-dipole interaction. To achieve this, the photoelectron continuum is expressed in terms of point dipole wavefunctions. The results of this model are then compared to experimental results from CN− and SO− photodetachment. In both cases, predicted angular distributions are closer to experimental values when incorporating a point dipole potential. Although the point dipole approach improves upon standard prediction techniques, it is still an approximation and can be further improved by using a physical dipole model in the future, allowing for adjustable charge separation between the two poles.
Language
English (en)
Chair and Committee
Richard Mabbs
Recommended Citation
Hart, C. Annie, "Dipole Effects in the Angular Distributions of Photoelectron Spectroscopy" (2023). Arts & Sciences Electronic Theses and Dissertations. 3165.
https://openscholarship.wustl.edu/art_sci_etds/3165