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Theoretical simulations of oxygen K-edge resonant inelastic x-ray scattering of kaolinite
Stockholm University, Faculty of Science, Department of Physics.
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Number of Authors: 12
2017 (English)In: Physical Review B, ISSN 2469-9950, E-ISSN 2469-9969, Vol. 95, no 14, article id 144301Article in journal (Refereed) Published
Abstract [en]

Near-edge x-ray absorption fine structure (NEXAFS) and resonant inelastic x-ray scattering (RIXS) measurements at the oxygen K edge were combined with theoretical spectrum simulations, based on periodic density functional theory and nuclear quantum dynamics, to investigate the electronic structure and chemical bonding in kaolinite Al2Si2O5(OH)(4). We simulated NEXAFS spectra of all crystallographically inequivalent oxygen atoms in the crystal and RIXS spectra of the hydroxyl groups. Detailed insight into the ground-state potential energy surface of the electronic states involved in the RIXS process were accessed by analyzing the vibrational excitations, induced by the core excitation, in quasielastic scattering back to the electronic ground state. In particular, we find that the NEXAFS pre-edge is dominated by features related to OH groups within the silica and alumina sheets, and that the vibrational progression in RIXS can be used to selectively probe vibrational modes of this subclass of OH groups. The signal is dominated by the OH stretching mode, but also other lower vibrational degrees of freedom, mainly hindered rotational modes, contribute to the RIXS signal.

Place, publisher, year, edition, pages
2017. Vol. 95, no 14, article id 144301
National Category
Physical Sciences
Research subject
Chemical Physics
Identifiers
URN: urn:nbn:se:su:diva-143605DOI: 10.1103/PhysRevB.95.144301ISI: 000399382500002OAI: oai:DiVA.org:su-143605DiVA, id: diva2:1104004
Available from: 2017-05-31 Created: 2017-05-31 Last updated: 2018-03-15Bibliographically approved
In thesis
1. Quantum chemical calculations of multidimensional dynamics probed in resonant inelastic X-ray scattering
Open this publication in new window or tab >>Quantum chemical calculations of multidimensional dynamics probed in resonant inelastic X-ray scattering
2018 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis is devoted to the theoretical study of the dynamical processes induced by light-matter interactions in molecules and molecular systems. To this end, the multidimensional nuclear dynamics probed in resonant inelastic X-ray scattering (RIXS) of small molecules, exemplified by H2O (g) and H2S (g), as well as more complex molecular systems, exemplified by NH3 (aq) and kaolinite clay, are modelled. The computational methodology consists of a combination of ab initio quantum chemistry calculations, quantum nuclear wave packet dynamics and in certain cases molecular dynamics modelling. This approach is used to simulate K-edge RIXS spectra and the theoretical results are evaluated against experimental measurements.

Specifically, the vibrational profile for decay back to the electronic ground state of the H2O molecule displays a vibrational selectivity introduced by the dynamics in the core-excited state. Simulation of the inelastic decay channel to the electronic |1b1-1,4a11> valence-excited state shows that the splitting of the spectral profile arises from the contribution of decay in the OH fragment. The character of the S1s-1 and S2p-1 core-excited states of the H2S molecule has been investigated and distinct similarities and differences with the H2O molecule have been identified. RIXS has also been used as a probe of the hydrogen bonding environment in aqueous ammonia and by detailed analysis of the valence orbitals of NH3 and water, the spectral profiles are explained. Finally, it is shown that vibrations of weakly hydrogen bonding OH are excited in RIXS decay to the electronic ground state in kaolinite. 

Place, publisher, year, edition, pages
Stockholm: Department of Physics, Stockholm University, 2018. p. 82
Keyword
quantum chemistry, X-ray spectroscopy, RASSCF, density functional theory, ultrafast nuclear dynamics
National Category
Atom and Molecular Physics and Optics
Research subject
Chemical Physics
Identifiers
urn:nbn:se:su:diva-154057 (URN)978-91-7797-173-3 (ISBN)978-91-7797-174-0 (ISBN)
Public defence
2018-05-04, sal FP41, hus 1, AlbaNova universitetscentrum, Roslagstullsbacken 21, Stockholm, 13:00 (English)
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Supervisors
Note

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 3: Manuscript. Paper 4: Manuscript.

Available from: 2018-04-11 Created: 2018-03-15 Last updated: 2018-04-04Bibliographically approved

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