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Combined Experimental and ab initio Multi Reference Configuration Interaction study of the Resonant Inelastic X-RayScattering spectrum of CO2
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and condensed matter physics.
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2014 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 118, no 35, 20163-20175 p.Article in journal (Refereed) Published
Abstract [en]

The fundamental problem of the symmetry breaking in the resonant inelastic X-ray scattering (RIXS) of the CO2 gas molecule is studied. The measurements were performed under catalytically relevant conditions within an in-house constructed reaction cell. The experimental RIXS plane is constructed from a sequence of resonances, covering the near-edge X-ray absorption fine structure (NEXAFS) spectrum up to 539 eV. The spectra show significant sensitivity with respect to the excitation frequency. The NEXAFS absorption spectrum, as well as the corresponding RIXS spectra, is interpreted with the aid of multireference configuration interaction (MRCI) theory. In this framework, the configuration interaction space spans the space of the intermediate and final states with single and single-double excitations. The dynamic character of the RIXS spectra is investigated by considering the electronic-nuclear vibrational coupling with the bending and antisymmetric stretching vibrations in the important intermediate excited states. In addition, the vibronic coupling mechanism involving the Renner-Teller effect and the core-hole localization pseudo-Jahn-Teller effect of the intermediate states is fully considered. The physical origin of the observed spectral features is discussed qualitatively and quantitatively in terms of individual core-to-valence excitations and valence-to-core decays, respectively. The computational protocol presented here, based on multireference wave function ab initio theory, serves as an important reference for future theoretical and experimental applications of RIXS spectroscopy.

Place, publisher, year, edition, pages
2014. Vol. 118, no 35, 20163-20175 p.
National Category
Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:uu:diva-209199DOI: 10.1021/jp505628yISI: 000341337700013OAI: oai:DiVA.org:uu-209199DiVA: diva2:656174
Available from: 2013-10-15 Created: 2013-10-15 Last updated: 2017-12-06Bibliographically approved
In thesis
1. In situ X-Ray Spectroscopy of Ethylene Epoxidation over Ag and studies of Li-ion batteries and Cu sulfidation
Open this publication in new window or tab >>In situ X-Ray Spectroscopy of Ethylene Epoxidation over Ag and studies of Li-ion batteries and Cu sulfidation
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis is based on experiments applying synchrotron based X-ray Absorption Spectroscopy(XAS) and Resonant Inelastic X-ray Scattering (RIXS) in the soft X-ray region to energy related systems. The main work of this thesis has been to develop a reaction cell that allowed for in situ XAS and RIXS investigations of the partial epoxidation of ethylene over a Ag catalyst at 1 atm and up to 250C. The developed in situ cell can be used in two sample modes: 1) the Ag catalyst is deposited directly onto the vacuum separating membrane with the reaction gases flowing beneath it or 2) a slightly compressed Ag powder sample is at a distance to the vacuum membrane with the reaction gases flowing between the Ag powder sample and the membrane.Both sample modes offers the total florescence yield, TFY, and the total electron yield, TEY, to be recorded simultaneously. By means of the developed in situ cell a number of oxygen species, residing in/on the Ag surface or in the Ag bulk, have been detected. We claim to detect adsorbed O2 under epoxidation conditions, as well as Ag–O–H groups. We are also able to monitor changes of the absorbed oxygen as we change the composition of the reaction gas feed. The first charging cycle of Li-ion batteries have been investigate by ex situ measurements on the cathode Li2-xMnSiO4 and the anode composite LixNi0:5TiOPO4/C . The initial crystalline material becomes amorphous due to lithiation during the first first charging. We find that the redox behaviors of these two states are significantly different. Sulfidation of natural copper oxides are is found to be strongly promoted when it is grown on the host metal by a disproportionation.

Place, publisher, year, edition, pages
Uppsala: Arkitektkopia, Uppsala, 2013. 64 p.
Keyword
In situ, XAS, RIXS, heterogeneous catalysis
National Category
Atom and Molecular Physics and Optics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-209204 (URN)
Public defence
2013-11-05, Å2005, Lägerhyddsvägen 1, Uppsala, 09:15 (English)
Opponent
Supervisors
Available from: 2013-10-15 Created: 2013-10-15 Last updated: 2013-10-16

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Kristiansen, PawDuda, Laurent-Claudius

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