Angle-resolved photoelectron spectroscopy of size-selected coinage metal cluster anions

Abstract: This thesis presents angle-resolved photoelectron measurements on anionic coinage metal clusters. The anisotropy parameter β of the spectra is extracted and β parameter curves are plotted against photoelectron momentum. Earlier experiments have shown a universal shape of the curves [10, 11, 12]. This universality has been explained recently by v. Issendorff [13]. The current measurements confirm this Issendorff model. Moreover, the model is then utilised to find the angular momentum character (f-type) of the orbitals involved in the premature shell closing observed for Cu−91 and Ag−91 . Additionally, mixing of angular momentum eigenstates is observed and the model is extended by the description of such mixing. Furthermore, measurements on gold clusters are the first that result in extended β parameter curves. Gold clusters exhibit the same universal shape of the β parameter curve, although special clusters (Au−20 and Au−34 ), remarkable for their unusually large band gap and their geometry, show deviating β parameter curves for the HOMO.
In the course of recording β parameter curves, many vibrational progressions, unseen before, are resolved. The vibrational frequencies are determined and electron affinity and vertical detachment energy are refined. In case of the Cu−5 cluster, DFT calculations are performed, which match experimental results if vibrational energies are globally rescaled by a factor of ≈ 1.05. The relation of vibrations and anisotropy is found to be more complex and is not explained (at least not in all cases) by the reduced photoelectron momentum

Object Details

• Location: Deutsche Nationalbibliothek Frankfurt am Main
• Extent: Online-Ressource
• Language: Englisch
• Notes: Universität Freiburg, Dissertation, 2023

Classification and Topics

• Keyword: Cluster ; Photoelektronenspektrum ; Winkelverteilung ; Cluster

Contributors, Places and Time

• Event: Veröffentlichung
• (where): Freiburg
• (who): Universität
• (when): 2023
• Creator: Weise, Lukas
• Contributor: Issendorff, Bernd von ; Issendorff, Bernd von ; Stienkemeier, Frank ; Albert-Ludwigs-Universität Freiburg. Fakultät für Mathematik und Physik

Further information

• DOI: 10.6094/UNIFR/237053
• URN: urn:nbn:de:bsz:25-freidok-2370536
• Rights: Open Access; Der Zugriff auf das Objekt ist unbeschränkt möglich.
• Last update: 25.03.2025, 1:56 PM CET