skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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

Abstract

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 dissociationmore » on the timescale of the O 1s core hole lifetime, which is strongly affected by the initial state hydrogen bonding configuration.« less

Authors:
; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
Advanced Light Source Division
OSTI Identifier:
971354
Report Number(s):
LBNL-2309E
Journal ID: ISSN 0368-2048; JESRAW; TRN: US1001166
DOE Contract Number:
DE-AC02-05CH11231
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Electron Spectroscopy and Related Phenomena; Related Information: Journal Publication Date: March 2009 online
Country of Publication:
United States
Language:
English
Subject:
36; BONDING; CONFIGURATION; DISSOCIATION; ELECTRONIC STRUCTURE; EMISSION SPECTROSCOPY; HYDROGEN; LIFETIME; RESOLUTION; SPECTRA; SPECTROSCOPY; SYNCHROTRON RADIATION; THERMODYNAMICS; WATER; WINDOWS; X-RAY SPECTROMETERS; water, RIXS, x-ray emission

Citation Formats

Weinhardt, L., Fuchs, O., Blum, M., Bär, M., Weigand, M., Denlinger, J.D., Zubavichus, Y., Zharnikov, M., Grunze, M., Heske, C., and Umbach, E.. Resonant x-ray emission spectroscopy of liquid water: novel instrumentation, high resolution, and the"map" approach. United States: N. p., 2008. Web.
Weinhardt, L., Fuchs, O., Blum, M., Bär, M., Weigand, M., Denlinger, J.D., Zubavichus, Y., Zharnikov, M., Grunze, M., Heske, C., & Umbach, E.. Resonant x-ray emission spectroscopy of liquid water: novel instrumentation, high resolution, and the"map" approach. United States.
Weinhardt, L., Fuchs, O., Blum, M., Bär, M., Weigand, M., Denlinger, J.D., Zubavichus, Y., Zharnikov, M., Grunze, M., Heske, C., and Umbach, E.. Tue . "Resonant x-ray emission spectroscopy of liquid water: novel instrumentation, high resolution, and the"map" approach". United States. doi:. https://www.osti.gov/servlets/purl/971354.
@article{osti_971354,
title = {Resonant x-ray emission spectroscopy of liquid water: novel instrumentation, high resolution, and the"map" approach},
author = {Weinhardt, L. and Fuchs, O. and Blum, M. and Bär, M. and Weigand, M. and Denlinger, J.D. and Zubavichus, Y. and Zharnikov, M. and Grunze, M. and Heske, C. and Umbach, E.},
abstractNote = {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.},
doi = {},
journal = {Journal of Electron Spectroscopy and Related Phenomena},
number = ,
volume = ,
place = {United States},
year = {Tue Jun 17 00:00:00 EDT 2008},
month = {Tue Jun 17 00:00:00 EDT 2008}
}