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Resonant Inelastic X-ray Scattering of Rare-Earth and Copper Systems
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics.
2006 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Rare earths and copper systems were studied using X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). The use of monochromased synchrotron radiation and improved energy resolution for RIXS made possible to obtain valuable information on the electronic structure in 4f, 5f and 3d systems. Experimental results for rare-earths (Ho, Gd, Cm,U, Np, Pu) were analyzed by atomic multiplet theory based on the Hartree-Fock calculations.

The inelastic scattering structures in RIXS spectra at 5d edge of actinides found to be sensitive to actinide oxidation states in different systems. Comparison of experimental and calculated Cm 5d RIXS spectra gave direct information about valency of the 248-curium isotope in oxide.

Scientific understanding of processes that control chemical changes of radioactive species from spent fuel is improved by studying interactions of actinide ions (U, Np, Pu) with corroded iron surfaces. RIXS measurements at the actinide 5d edge indicate the reduction of U(VI), Np (V) and Pu (VI) to U(IV), Np(IV) and Pu (IV) by presence of iron ions.

This thesis is also addressed to the study of changes in the electronic structure of copper films during interaction with synthetic groundwater solutions. The surface modifications induced by chemical reactions of oxidized 100Å Cu films with Cl, SO42− and HCO3 ions in aqueous solutions with various concentrations were studied in-situ using XAS. It was shown that the pH value, the concentration of Cl ion and presence of HCO3 ion in the solutions strongly affect the speed of the corrosion reaction. The Cu 2p RIXS was used to distinguish between the species present on the copper surface while in contact with groundwater solution.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis , 2006. , p. 52
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 205
Keywords [en]
Physics, resonant inelastic X-ray scattering
Keywords [sv]
Fysik
Identifiers
URN: urn:nbn:se:uu:diva-7094ISBN: 91-554-6625-7 (print)OAI: oai:DiVA.org:uu-7094DiVA, id: diva2:168701
Public defence
2006-09-22, Häggsalen, Ångström Laboratory, Lägerhyddsvägen 1, Polacksbacken, Uppsala, 10:15 (English)
Opponent
Supervisors
Available from: 2006-09-01 Created: 2006-09-01 Last updated: 2010-03-10Bibliographically approved
List of papers
1. Influence of Hydrogen on Properties of Rare-Earth Hydrides Studied by Resonant Inelastic X-ray Scattering spectroscopy
Open this publication in new window or tab >>Influence of Hydrogen on Properties of Rare-Earth Hydrides Studied by Resonant Inelastic X-ray Scattering spectroscopy
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2006 (English)In: AIP Conference Proc., ISSN 0094-243X, Vol. 837, p. 255-237Article in journal (Refereed) Published
National Category
Natural Sciences
Identifiers
urn:nbn:se:uu:diva-94729 (URN)
Available from: 2006-09-01 Created: 2006-09-01 Last updated: 2016-04-29
2. Electronic Structure of Gd Hydrides Studied by Resonant Inelastic Soft X-ray Scattering
Open this publication in new window or tab >>Electronic Structure of Gd Hydrides Studied by Resonant Inelastic Soft X-ray Scattering
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2004 (English)In: Journal of electron Spectroscopy and Related Phenomena, Vol. 137-140, p. 487-489Article in journal (Refereed) Published
National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-94730 (URN)
Available from: 2006-09-01 Created: 2006-09-01 Last updated: 2012-03-07Bibliographically approved
3. Resonant inelastic x-ray scattering of curium oxide
Open this publication in new window or tab >>Resonant inelastic x-ray scattering of curium oxide
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2007 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 75, no 11, p. 115107-Article in journal (Refereed) Published
Abstract [en]

The measurements on radioactive actinide isotopes (curium-248) were performed using very small sample quantities (micrograms) to minimize the sample activity. Resonant inelastic x-ray scattering (RIXS) spectra of curium oxide at the Cm 5d edge were measured for the first time. RIXS data are compared with theoretical calculations using atomic multiplet theory. The results indicate that isotope curium -248 in the curium oxide sample has oxidation state III due to the best agreement with RIXS calculations for Cm (III) instead of those for Cm (IV).

National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-94736 (URN)10.1103/PhysRevB.75.115107 (DOI)000245329600035 ()
Available from: 2006-09-01 Created: 2006-09-01 Last updated: 2017-12-14
4. Resonant Inelastic Soft X-ray Studies of Uranium (VI) Reduction on Iron Surfaces
Open this publication in new window or tab >>Resonant Inelastic Soft X-ray Studies of Uranium (VI) Reduction on Iron Surfaces
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2004 In: MRS Symp. Proc., Vol. 807, p. 113-118Article in journal (Refereed) Published
Identifiers
urn:nbn:se:uu:diva-94732 (URN)
Available from: 2006-09-01 Created: 2006-09-01Bibliographically approved
5. Immobilization of UO2+2 and NpO+2 Carbonate in Groundwater through Reduction on Corroding Iron
Open this publication in new window or tab >>Immobilization of UO2+2 and NpO+2 Carbonate in Groundwater through Reduction on Corroding Iron
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Manuscript (Other academic)
Identifiers
urn:nbn:se:uu:diva-94733 (URN)
Available from: 2006-09-01 Created: 2006-09-01 Last updated: 2010-01-13Bibliographically approved
6. Studies of Actinides Reduction on Iron Surface by means of Resonant Inelastic X-ray Scattering
Open this publication in new window or tab >>Studies of Actinides Reduction on Iron Surface by means of Resonant Inelastic X-ray Scattering
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Manuscript (Other academic)
Identifiers
urn:nbn:se:uu:diva-94734 (URN)
Available from: 2006-09-01 Created: 2006-09-01 Last updated: 2010-01-13Bibliographically approved
7. Resonant Inelastic X-ray Scattering Study of Copper Compounds and Minerals at Cu L3 edge
Open this publication in new window or tab >>Resonant Inelastic X-ray Scattering Study of Copper Compounds and Minerals at Cu L3 edge
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Manuscript (Other academic)
Identifiers
urn:nbn:se:uu:diva-94735 (URN)
Available from: 2006-09-01 Created: 2006-09-01 Last updated: 2010-01-13Bibliographically approved
8. Resonant inelastic x-ray scattering of curium oxide
Open this publication in new window or tab >>Resonant inelastic x-ray scattering of curium oxide
Show others...
2007 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 75, no 11, p. 115107-Article in journal (Refereed) Published
Abstract [en]

The measurements on radioactive actinide isotopes (curium-248) were performed using very small sample quantities (micrograms) to minimize the sample activity. Resonant inelastic x-ray scattering (RIXS) spectra of curium oxide at the Cm 5d edge were measured for the first time. RIXS data are compared with theoretical calculations using atomic multiplet theory. The results indicate that isotope curium -248 in the curium oxide sample has oxidation state III due to the best agreement with RIXS calculations for Cm (III) instead of those for Cm (IV).

National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-94736 (URN)10.1103/PhysRevB.75.115107 (DOI)000245329600035 ()
Available from: 2006-09-01 Created: 2006-09-01 Last updated: 2017-12-14
9. Suppression of Copper Corrosion in Groundwaters Observed by In-situ X-ray Absorption Spectroscopy
Open this publication in new window or tab >>Suppression of Copper Corrosion in Groundwaters Observed by In-situ X-ray Absorption Spectroscopy
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In: NatureArticle in journal (Refereed) Submitted
Identifiers
urn:nbn:se:uu:diva-94737 (URN)
Available from: 2006-09-01 Created: 2006-09-01Bibliographically approved

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