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A study of the water molecule using frequency control over nuclear dynamics in resonant X-ray scattering
Stockholm University, Faculty of Science, Department of Physics.
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Number of Authors: 15
2017 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 19, no 30, p. 19573-19589Article in journal (Refereed) Published
Abstract [en]

In this combined theoretical and experimental study we report a full analysis of the resonant inelastic X-ray scattering (RIXS) spectra of H2O, D2O and HDO. We demonstrate that electronically-elastic RIXS has an inherent capability to map the potential energy surface and to perform vibrational analysis of the electronic ground state in multimode systems. We show that the control and selection of vibrational excitation can be performed by tuning the X-ray frequency across core-excited molecular bands and that this is clearly reflected in the RIXS spectra. Using high level ab initio electronic structure and quantum nuclear wave packet calculations together with high resolution RIXS measurements, we discuss in detail the mode coupling, mode localization and anharmonicity in the studied systems.

Place, publisher, year, edition, pages
2017. Vol. 19, no 30, p. 19573-19589
National Category
Physical Sciences
Research subject
Chemical Physics
Identifiers
URN: urn:nbn:se:su:diva-147090DOI: 10.1039/c7cp01215bISI: 000407053000006PubMedID: 28352891OAI: oai:DiVA.org:su-147090DiVA, id: diva2:1148766
Available from: 2017-10-12 Created: 2017-10-12 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)
Opponent
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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