Resonant x-ray emission spectroscopy of liquid water: novel instrumentation, high resolution, and the"map" approach

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Techniques to study the electronic structure of liquids are rare. Most recently, resonant x-ray emission spectroscopy (XES) has been shown to be an extremely versatile spectroscopy to study both occupied and unoccupied electronic states for liquids in thermodynamic equilibrium. However, XES requires high-brilliance soft x-ray synchrotron radiation and poses significant technical challenges to maintain a liquid sample in an ultra-high vacuum environment. Our group has therefore developed and constructed a novel experimental setup for the study of liquids, with the long-term goal of investigating the electronic structure of biological systems in aqueous environments. We have developed a flow-through liquid cell ... continued below

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Weinhardt, L.; Fuchs, O.; Blum, M.; Bär, M.; Weigand, M.; Denlinger, J.D. et al. June 17, 2008.

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Techniques to study the electronic structure of liquids are rare. Most recently, resonant x-ray emission spectroscopy (XES) has been shown to be an extremely versatile spectroscopy to study both occupied and unoccupied electronic states for liquids in thermodynamic equilibrium. However, XES requires high-brilliance soft x-ray synchrotron radiation and poses significant technical challenges to maintain a liquid sample in an ultra-high vacuum environment. Our group has therefore developed and constructed a novel experimental setup for the study of liquids, with the long-term goal of investigating the electronic structure of biological systems in aqueous environments. We have developed a flow-through liquid cell in which the liquid is separated from vacuum by a thin Si3N4 or SiC window and which allows a precise control of temperature. This approach has significant advantages compared to static liquids cells used in the past. Furthermore, we have designed a dedicated high-transmission, high-resolution soft x-ray spectrometer. The high transmission makes it possible to measure complete resonant XES"maps" in less than an hour, giving unprecedented detailed insight into the electronic structure of the investigated sample. Using this new equipment we have investigated the electronic structure of liquid water. Furthermore, our XES spectra and maps give information about ultra-fast dissociation on the timescale of the O 1s core hole lifetime, which is strongly affected by the initial state hydrogen bonding configuration.

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  • Journal Name: Journal of Electron Spectroscopy and Related Phenomena; Related Information: Journal Publication Date: March 2009 online

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  • Report No.: LBNL-2309E
  • Grant Number: DE-AC02-05CH11231
  • Office of Scientific & Technical Information Report Number: 971354
  • Archival Resource Key: ark:/67531/metadc930226

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  • June 17, 2008

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  • Nov. 13, 2016, 7:26 p.m.

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  • Jan. 4, 2017, 4:39 p.m.

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Weinhardt, L.; Fuchs, O.; Blum, M.; Bär, M.; Weigand, M.; Denlinger, J.D. et al. Resonant x-ray emission spectroscopy of liquid water: novel instrumentation, high resolution, and the"map" approach, article, June 17, 2008; Berkeley, California. (digital.library.unt.edu/ark:/67531/metadc930226/: accessed July 18, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.