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Title: Fast atom bombardment mass spectrometry of clusters and adducts based on uranium and lanthanides
Author: Read, Paul Anthony
ISNI:       0000 0001 3510 3294
Awarding Body: University of Warwick
Current Institution: University of Warwick
Date of Award: 1993
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The fast atom bombardment, FAB, of salts of uranium, the lanthanides and related metals yield long, well defined series of cations of metal-oxygen clusters, < MxOv > with x up to 30-40. Up to seven values of y are associated with each value of x, but in each set of clusters there is usually a well-defined ion of maximum abundance. These series consist of regular patterns of clusters whose relative stabilities and structures can be directly related to reported solid state structures, demonstrating the strong Influences of solid state processes at the molecular level. Thus, direct correlations are found between these metal-oxygen clusters and the complex metal-oxide phases exhibited by the actinide and lanthanide metals. The mass spectral and collision-induced decomposition < CID ) spectral data obtained for many of these clusters feature ion abundances depending on cluster size, and a pronounced odd/even alternation, both of which are interpreted in terms of the electronic and geometrical structures of the clusters. Similar trends are also demonstrated for series based on the general formula (UxCLn)- with x up to 13. Conditions of sample preparation < matrix, source pressure, etc. > are described for the achievement of maximal cluster formation and fragmentation reactions. The fabrication and deployment of a 'split' FAB source is described which enables the simultaneous bombardment of two samples to yield 'mixed' clusters. The FAB spectra of a variety of uranyl complexes containing biologically important molecules, such as peptides, demonstrate the sequential loss of the ligands. The inter-relationship between their mode of fragmentation, and the extent of ligand coordination, as well as their relative ion abundances is described.
Supervisor: Not available Sponsor: Not available
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available
Keywords: QC Physics ; QD Chemistry