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Photochemistry and Ultrafast Dynamics of Mass-selected Multinuclear Coinage Metal Complexes Studied by Electronic Photodissociation Ion Spectroscopy in an Ion Trap

  • Subject of this thesis is the investigation of photo-induced ultrafast elementary processes within the electronic excited-state manifold in mass-selected multinuclear coinage metal complexes (CMCs) in the gas phase. The chief objective is to ascertain how the intramolecular deactivation dynamics and gas phase reactivity are influenced by so-called metallophilic interactions between multiple d^10/d^8 metal centers, which in turn give rise to metal-delocalized electronic transitions. To this end, suitable molecular precursor ions were transferred into the gas phase by electrospray ionization (ESI) and subsequently isolated, activated, and finally analyzed in a Paul-type quadrupole ion trap (QIT) mass spectrometer. The QIT is modified to accept UV/Vis/NIR irradiation from a femtosecond laser setup. By combining several ion trap-based ion activation techniques and electronic photodissociation (PD) spectroscopy, the fragmentation pathways, as well as intrinsic optical properties (electronic PD spectra) of ionic CMCs are explored. In addition, the unconventional time-resolved transient photodissociation (t-PD) method, based on a femtosecond pump-probe excitation scheme, was employed for the first time on CMC ions in isolation, in order to elucidate their intrinsic photodynamics. This thesis mainly comprises five publications, covering the mass spectrometric and laser spectroscopic characterization of multinuclear Ag(I), Au(I), and Pt(II) based ionic complexes.
Author:Sebastian KruppaORCiD
URN (permanent link):urn:nbn:de:hbz:386-kluedo-62586
Advisor:Christoph RiehnORCiD
Document Type:Doctoral Thesis
Language of publication:English
Publication Date:2021/02/11
Year of Publication:2021
Publishing Institute:Technische Universität Kaiserslautern
Granting Institute:Technische Universität Kaiserslautern
Acceptance Date of the Thesis:2021/01/15
Date of the Publication (Server):2021/02/16
GND-Keyword:Femtosekundenspektroskopie; Ionenfalle; Münzmetall; Photodissoziation; Silberkomplexe
Number of page:258
Faculties / Organisational entities:Fachbereich Chemie
DDC-Cassification:5 Naturwissenschaften und Mathematik / 540 Chemie
PACS-Classification (physics):30.00.00 ATOMIC AND MOLECULAR PHYSICS
Licence (German):Creative Commons 4.0 - Namensnennung, nicht kommerziell, keine Bearbeitung (CC BY-NC-ND 4.0)