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A High-resolution Study of Resonant Auger Decay Processes in N2O After Core Electron Excitation from Terminal Nitrogen, Central Nitrogen and Oxygen Atoms to the 3π LUMO
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics, Physics V.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics, Physics V.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics, Physics V.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics, Physics V.
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2007 (English)In: Journal of Physics B: Atomic, Molecular and Optical Physics, ISSN 0953-4075, E-ISSN 1361-6455, Vol. 40, no 17, 3357-3365 p.Article in journal (Refereed) Published
Abstract [en]

Decay spectra of N2O following excitation to the N terminal (Nt) → π*, N central (Nc) → π* and O is → π* intermediate states are reported. The final states reached after participator decay show resonant enhancement consistent with a local-density-of-states analysis based on the Mulliken population of the valence molecular orbitals. In particular, the X-state is resonantly enhanced mostly after excitation from the Nt 1s and the O Is core levels to the π*, while the B-state is mostly enhanced following the excitation of the Nc Is → π* intermediate state. Below the Nt Is threshold, the lowest lying peak related to spectator decay falls at lower binding energy than the highest lying participator peak. This can be attributed to a particularly strong screening effect exerted by the excited electron in the LUMO.

Place, publisher, year, edition, pages
2007. Vol. 40, no 17, 3357-3365 p.
Keyword [en]
Nitrogen protoxide, Frontier orbital, Inner-shell excitation, Triatomic molecule, Inorganic compounds, Electron charge distribution, Binding energy, Core levels, Density of states, Molecular orbital, Excitation, Auger effect
National Category
Physical Sciences
Identifiers
URN: urn:nbn:se:uu:diva-97316DOI: 10.1088/0953-4075/40/17/004ISI: 000249223500007OAI: oai:DiVA.org:uu-97316DiVA: diva2:172195
Available from: 2008-05-15 Created: 2008-05-15 Last updated: 2017-12-14Bibliographically approved
In thesis
1. Structure and Dynamics of Core-Excited Species
Open this publication in new window or tab >>Structure and Dynamics of Core-Excited Species
2008 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In this thesis we have performed core-electron spectroscopy studies of gas phase molecular systems starting with smaller diatomic, continuing with triatomic and extending our research to more complex polyatomic ones. We can subdivide the results presented here into two categories: the first one focusing on electronic fine structure and effect of the chemical bonds on molecular core-levels and the other one dealing with nuclear dynamics induced by creation of a core hole. In our research we have mostly used synchrotron radiation based techniques such as X-ray Photoelectron (XPS), X-ray Absorption (XAS), normal and Resonant Auger (AES and RAS, respectively) and Energy-Selected Auger Electron PhotoIon COincidence (ES-AEPICO) spectroscopies.

We have demonstrated that resonant Auger spectroscopy can be used to aid interpretation of the features observed in XAS for Rydberg structures in the case of Cl2 and C1s−1π*1 states of allene molecules. The combined use of high-resolution spectroscopy with ab initio calculations can help the interpretation of strongly overlapped spectral features and disentangle their complex profiles. This approach enabled us to determine the differences in the lifetimes for core-hole 2p sublevels of Cl2 which are caused by the presence of the chemical bond. We have shown that contribution in terms of the Mulliken population of valence molecular orbitals is a determining factor for resonant enhancement of different final states and fragmentation patterns reached after resonant Auger decays in N2O.

We have also performed a systematic study of the dependence of the C1s resonant Auger kinetic energies on the presence of different substituents in CH3X compounds. For the first time we have studied possible isomerization reaction induced by core excitation of acetylacetone. We could observe a new spectral feature in the resonant Auger decay spectra which we interpreted as a signature of core-excitation-induced keto-enol tautomerism.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2008. x, 68 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 442
Keyword
Physics, Synchrotron radiation, X-ray Photoelectron Spectroscopy (XPS), X-ray Absorption Spectroscopy (XAS), Resonant Auger Spectroscopy (RAS), Auger Electron Spectroscopy (AES), Energy-Selected Auger Electron PhotoIon COincidence (ES-AEPICO), core excitation, core ionization, linear free energy relationships (LFER), molecular-field splitting, substituent effects, nuclear dynamics, isomerization, Cl2, N2O, methane derivatives, allene, acetylacetone, Fysik
Identifiers
urn:nbn:se:uu:diva-8904 (URN)978-91-554-7223-8 (ISBN)
Public defence
2008-06-05, Polhemsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 10:15
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Available from: 2008-05-15 Created: 2008-05-15Bibliographically approved

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