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Electronic Structure and Core-Hole Dynamics of Ozone: Synchrotron-radiation based studies and ab-initio calculations
Uppsala University, Teknisk-naturvetenskapliga vetenskapsområdet, Physics, Department of Physics.
2003 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The electronic structure of the ozone molecule O3 has been studied with spectroscopy techniques and computations. The investigation was focused on O3 in a core-hole state. The electronic configuration and the nuclear dynamics have been found to be highly correlated.

This electron correlation is mapped out for the two chemically different sites in the molecule: the central and the terminal oxygen. The energy difference between the corresponding core orbitals is 4.58 eV, which allows for site-selective core ionization and core excitation.

The influence of the core-hole site on the electronic structure is substantial, which is shown with ion and electron spectroscopy data and ab-initio quantum chemical computations. Moreover, the induced nuclear motion differs considerably for the two core-hole sites.

One of the core-excited states is proven to be ultra-fast dissociative. An analysis of the data with a formalism for two-body dissociation disclosed the localized character of core excitation. The symmetry-equivalent terminal-oxygen core orbitals do have very little overlap, so that a delocalized model for the core excitation becomes inadequate.

Moreover, core-excitation opens up a decay channel to a valence-ionized state that has not been observed with photoionization. The reason for this state to have low cross section for photoionization is illuminated with a CASSCF computation of the electronic configuration. The configuration of the state was found to be very distinct from the ground state configuration.

Another effect of configuration-interaction was found in MRCI computations of the core- ionized states. Several local minima with distinct electronic configurations could be identified.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis , 2003. , p. 55
Series
Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1104-232X ; 921
Keywords [en]
Physics
Keywords [sv]
Fysik
National Category
Physical Sciences
Identifiers
URN: urn:nbn:se:uu:diva-3914ISBN: 91-554-5842-4 (print)OAI: oai:DiVA.org:uu-3914DiVA, id: diva2:163895
Public defence
2004-01-24, Häggsalen, Ångströmlaboratoratoriet, Lägerhyddsvägen 1, Uppsala, 10:15
Opponent
Supervisors
Available from: 2003-12-16 Created: 2003-12-16Bibliographically approved
List of papers
1. Femtosecond dissociation of ozone studied by the Auger Doppler effect: ----
Open this publication in new window or tab >>Femtosecond dissociation of ozone studied by the Auger Doppler effect: ----
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2001 (English)In: Journal of Chemical Physics, ISSN -----, Vol. 115, no 8, p. 3614-3620Article in journal (Refereed) Published
National Category
Natural Sciences
Identifiers
urn:nbn:se:uu:diva-91227 (URN)
Available from: 2003-12-16 Created: 2003-12-16 Last updated: 2012-04-02Bibliographically approved
2. Experimental study of photoionization of ozone in the 12 to 21 eV region: -----
Open this publication in new window or tab >>Experimental study of photoionization of ozone in the 12 to 21 eV region: -----
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2001 In: Journal of Chemical Physics, ISSN -----, Vol. 115, no 11, p. 5041-5046Article in journal (Refereed) Published
Identifiers
urn:nbn:se:uu:diva-91228 (URN)
Available from: 2003-12-16 Created: 2003-12-16Bibliographically approved
3. The dynamic Auger-Doppler effect in HF and DF: control of fragment velocities in femtosecond dissociation through photon energy detuning
Open this publication in new window or tab >>The dynamic Auger-Doppler effect in HF and DF: control of fragment velocities in femtosecond dissociation through photon energy detuning
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2002 In: Chemical Physics Letters, ISSN -----, Vol. 354, no -----, p. 382-388Article in journal (Refereed) Published
Identifiers
urn:nbn:se:uu:diva-91229 (URN)
Available from: 2003-12-16 Created: 2003-12-16Bibliographically approved
4. Valence photoionization and resonant core excitation of ozone: experimental and theoretical study of the ~C-state of O3+
Open this publication in new window or tab >>Valence photoionization and resonant core excitation of ozone: experimental and theoretical study of the ~C-state of O3+
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2003 In: Chemical Physics Letters, ISSN -----, Vol. 375, no -----, p. 76-83Article in journal (Refereed) Published
Identifiers
urn:nbn:se:uu:diva-91230 (URN)
Available from: 2003-12-16 Created: 2003-12-16Bibliographically approved
5. Core excitation in O3 localized to one chemical bond: -----
Open this publication in new window or tab >>Core excitation in O3 localized to one chemical bond: -----
In: Physical Review LettersArticle in journal (Refereed) Submitted
Identifiers
urn:nbn:se:uu:diva-91231 (URN)
Available from: 2003-12-16 Created: 2003-12-16Bibliographically approved
6. Electronic structure of core-ionized ozone - Computation and Experiment
Open this publication in new window or tab >>Electronic structure of core-ionized ozone - Computation and Experiment
Manuscript (Other academic)
Identifiers
urn:nbn:se:uu:diva-91232 (URN)
Available from: 2003-12-16 Created: 2003-12-16 Last updated: 2010-01-13Bibliographically approved
7. Analytic Expressions for Ion Profiles from Ion Coincidence Data: -----
Open this publication in new window or tab >>Analytic Expressions for Ion Profiles from Ion Coincidence Data: -----
Manuscript (Other academic)
Identifiers
urn:nbn:se:uu:diva-91233 (URN)
Available from: 2003-12-16 Created: 2003-12-16 Last updated: 2010-01-13Bibliographically approved
8. Fragmentation of core-excited O3: -----
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Manuscript (Other academic)
Identifiers
urn:nbn:se:uu:diva-91234 (URN)
Available from: 2003-12-16 Created: 2003-12-16 Last updated: 2010-01-13Bibliographically approved
9. Selective dissociation of ozone probed by coincidence measurements between energy selected photoelectrons and fragment ions: -----
Open this publication in new window or tab >>Selective dissociation of ozone probed by coincidence measurements between energy selected photoelectrons and fragment ions: -----
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Manuscript (Other academic)
Identifiers
urn:nbn:se:uu:diva-91235 (URN)
Available from: 2003-12-16 Created: 2003-12-16 Last updated: 2010-01-13Bibliographically approved

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