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Reabsorption of Soft X-Ray Emission at High X-Ray Free-Electron Laser Fluences
Stockholm University, Faculty of Science, Department of Physics. SLAC National Accelerator Laboratory, USA.
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2014 (English)In: Physical Review Letters, ISSN 0031-9007, E-ISSN 1079-7114, Vol. 113, no 15, 153002- p.Article in journal (Refereed) Published
Abstract [en]

We report on oxygen K-edge soft x-ray emission spectroscopy from a liquid water jet at the Linac Coherent Light Source. We observe significant changes in the spectral content when tuning over a wide range of incident x-ray fluences. In addition the total emission yield decreases at high fluences. These modifications result from reabsorption of x-ray emission by valence-excited molecules generated by the Auger cascade. Our observations have major implications for future x-ray emission studies at intense x-ray sources. We highlight the importance of the x-ray pulse length with respect to the core-hole lifetime.

Place, publisher, year, edition, pages
2014. Vol. 113, no 15, 153002- p.
National Category
Physical Sciences
URN: urn:nbn:se:su:diva-110198DOI: 10.1103/PhysRevLett.113.153002ISI: 000344245600005OAI: diva2:769967


Available from: 2014-12-09 Created: 2014-12-08 Last updated: 2015-09-18Bibliographically approved
In thesis
1. X-ray scattering and spectroscopy of supercooled water and ice
Open this publication in new window or tab >>X-ray scattering and spectroscopy of supercooled water and ice
2014 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis presents experimental studies of water and ice at near-atmospheric pressures using intense x-rays only accessible at synchrotrons and free-electron lasers. In particular, it focuses on the deeply supercooled, metastable state and its implications on ice nucleation.

The local structure of the liquid phase was studied by x-ray scattering over a wide temperature range extending from 339 K down to 227 K. In order to be able to study the deeply supercooled liquid, micron-sized water droplets were evaporatively cooled in vacuum and probed by ultrashort x-ray pulses. This is to date the lowest temperature at which measurements of the structure have been performed on bulk liquid water cooled from room temperature. Upon deep supercooling, the structure evolved toward that of a low-density liquid with local tetrahedral coordination. At ~230 K, where the low-density liquid structure started to dominate, the number of droplets containing ice nuclei increased rapidly. The estimated nucleation rate suggests that there is a “fragile-to-strong” transition in the dynamics of the liquid below 230 K, and its implications on water structure are discussed.

Similarly, the electronic structure of deeply supercooled water was studied by x-ray emission spectroscopy down to 222 K, but the spectral changes expected from the structural transformation remained absent and explanations are discussed. At high fluence, the non-linear dependence of the x-ray emission yield indicated that there were high valence hole densities created during the x-ray pulse length due to Auger cascades, resulting in reabsorption of the x-ray emission.

Finally, the hydrogen-bonded network in water was studied by x-ray absorption spectroscopy and compared to various ices. It was found that the pre-edge absorption cross-section, which is associated with distorted hydrogen bonds, could be minimized for crystalline ice grown on a hydrophobic BaF2(111) surface with low concentration of nucleation centers.

Place, publisher, year, edition, pages
Stockholm: Department of Physics, Stockholm Univeristy, 2014. 148 p.
supercooled water, ice, x-ray scattering, x-ray spectroscopy, free-electron laser
National Category
Physical Chemistry
Research subject
Chemical Physics
urn:nbn:se:su:diva-103009 (URN)978–91–7447–902–7 (ISBN)
Public defence
2014-05-30, FA32, AlbaNova Universitetscentrum, Roslagstullsbacken 21, Stockholm, 10:15 (English)

At the time of the doctoral defense, the following papers were unpublished and had a status as follows: Paper 2: Manuscript. Paper 3: Manuscript. Paper 4: Manuscript. Paper 5: Manuscript. Paper 6: Manuscript.

Available from: 2014-05-08 Created: 2014-04-26 Last updated: 2015-09-18Bibliographically approved

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Sellberg, Jonas A.Schlesinger, DanielPettersson, Lars G. M.Nilsson, Anders
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