Studies of reactive intermediates with synchrotron radiation
Studies of reactive intermediates with synchrotron radiation
Synchrotron radiation, with its continuously variable photon energy, greatly extends the range of photoelectron spectroscopic experiments that may be performed on a sample. However, few such studies have been executed on short-lived, reactive molecules. In this thesis, the design, construction and operation of a new photoelectron (PE) spectrometer for use with synchrotron radiation at Daresbury Laboratories are described, and the initial results obtained for a selective of reactive species are presented.
The spectrometer incorporates a powerful differential pumping system, to minimise contamination by the samples under study, and a three-element electron lens for efficient transmission of photoelectrons into a hemispherical electrostatic analyser. The entire vacuum system may be rotated around the axis of the polarised photon beam, so that angle-resolved photoelectron measurements may be made.
The first results obtained, on sulphur monoxide, carbon monosulphide and molecular oxygen in its first excited state, have revealed complex autoionisation structures in the constant ironic state spectra, most of which are assigned to particular Rydberg states in these molecules. Photoelectron spectra recorded at resonant photon energies display extended vibrational structure in some bands, allowing the determination of accurate spectroscopic constants for the corresponding ionic states. Near-threshold photoelectron studies have yielded high-resolution spectra containing a considerable amount of structure. Additionally, some preliminary experiments on ozone have provided some high resolution near-threshold PE spectra, and also constant ionic state spectra that indicate for the first time the existence of some weakly autoionising Rydberg states. Suggestions are made for ways in which the apparatus may be improved, and some future experiments are proposed.
University of Southampton
1997
Wright, Andrew Edward
(1997)
Studies of reactive intermediates with synchrotron radiation.
University of Southampton, Doctoral Thesis.
Record type:
Thesis
(Doctoral)
Abstract
Synchrotron radiation, with its continuously variable photon energy, greatly extends the range of photoelectron spectroscopic experiments that may be performed on a sample. However, few such studies have been executed on short-lived, reactive molecules. In this thesis, the design, construction and operation of a new photoelectron (PE) spectrometer for use with synchrotron radiation at Daresbury Laboratories are described, and the initial results obtained for a selective of reactive species are presented.
The spectrometer incorporates a powerful differential pumping system, to minimise contamination by the samples under study, and a three-element electron lens for efficient transmission of photoelectrons into a hemispherical electrostatic analyser. The entire vacuum system may be rotated around the axis of the polarised photon beam, so that angle-resolved photoelectron measurements may be made.
The first results obtained, on sulphur monoxide, carbon monosulphide and molecular oxygen in its first excited state, have revealed complex autoionisation structures in the constant ironic state spectra, most of which are assigned to particular Rydberg states in these molecules. Photoelectron spectra recorded at resonant photon energies display extended vibrational structure in some bands, allowing the determination of accurate spectroscopic constants for the corresponding ionic states. Near-threshold photoelectron studies have yielded high-resolution spectra containing a considerable amount of structure. Additionally, some preliminary experiments on ozone have provided some high resolution near-threshold PE spectra, and also constant ionic state spectra that indicate for the first time the existence of some weakly autoionising Rydberg states. Suggestions are made for ways in which the apparatus may be improved, and some future experiments are proposed.
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Published date: 1997
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Local EPrints ID: 463079
URI: http://eprints.soton.ac.uk/id/eprint/463079
PURE UUID: 1d8cc639-0046-4466-8642-75df773a1e61
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Date deposited: 04 Jul 2022 20:43
Last modified: 04 Jul 2022 20:43
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Author:
Andrew Edward Wright
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