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Title: Revisiting the total ion yield x-ray absorption spectra of liquid water microjets

Abstract

Measurements of the total ion yield (TIY) x-ray absorption spectrum (XAS) of liquid water by Wilson et al. (2002 J. Phys.: Condens. Matter 14 L221 and 2001 J. Phys. Chem. B 105 3346) have been revisited in light of new experimental and theoretical efforts by our group. Previously, the TIY spectrum was interpreted as a distinct measure of the electronic structure of the liquid water surface. However, our new results indicate that the previously obtained spectrum may have suffered from as yet unidentified experimental artifacts. Although computational results indicate that the liquid water surface should exhibit a TIY-XAS that is fundamentally distinguishable from the bulk liquid XAS, the new experimental results suggest that the observable TIY-XAS is actually nearly identical in appearance to the total electron yield (TEY-)XAS, which is a bulk probe. This surprising similarity between the observed TIY-XAS and TEY-XAS likely results from large contributions from x-ray induced electron stimulated desorption of ions, and does not necessarily indicate that the electronic structure of the bulk liquid and liquid surface are identical.

Authors:
; ; ; ;
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
Chemical Sciences Division
OSTI Identifier:
927885
Report Number(s):
LBNL-189E
TRN: US0804744
DOE Contract Number:  
DE-AC02-05CH11231
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Physics: Condensed Matter; Journal Volume: 20; Journal Issue: 20; Related Information: Journal Publication Date: May 21, 2008
Country of Publication:
United States
Language:
English
Subject:
75; ABSORPTION; ABSORPTION SPECTRA; DESORPTION; ELECTRONIC STRUCTURE; ELECTRONS; WATER

Citation Formats

Saykally, Richard J, Cappa, Chris D., Smith, Jared D., Wilson, Kevin R., and Saykally, Richard J.. Revisiting the total ion yield x-ray absorption spectra of liquid water microjets. United States: N. p., 2008. Web.
Saykally, Richard J, Cappa, Chris D., Smith, Jared D., Wilson, Kevin R., & Saykally, Richard J.. Revisiting the total ion yield x-ray absorption spectra of liquid water microjets. United States.
Saykally, Richard J, Cappa, Chris D., Smith, Jared D., Wilson, Kevin R., and Saykally, Richard J.. Sat . "Revisiting the total ion yield x-ray absorption spectra of liquid water microjets". United States. doi:. https://www.osti.gov/servlets/purl/927885.
@article{osti_927885,
title = {Revisiting the total ion yield x-ray absorption spectra of liquid water microjets},
author = {Saykally, Richard J and Cappa, Chris D. and Smith, Jared D. and Wilson, Kevin R. and Saykally, Richard J.},
abstractNote = {Measurements of the total ion yield (TIY) x-ray absorption spectrum (XAS) of liquid water by Wilson et al. (2002 J. Phys.: Condens. Matter 14 L221 and 2001 J. Phys. Chem. B 105 3346) have been revisited in light of new experimental and theoretical efforts by our group. Previously, the TIY spectrum was interpreted as a distinct measure of the electronic structure of the liquid water surface. However, our new results indicate that the previously obtained spectrum may have suffered from as yet unidentified experimental artifacts. Although computational results indicate that the liquid water surface should exhibit a TIY-XAS that is fundamentally distinguishable from the bulk liquid XAS, the new experimental results suggest that the observable TIY-XAS is actually nearly identical in appearance to the total electron yield (TEY-)XAS, which is a bulk probe. This surprising similarity between the observed TIY-XAS and TEY-XAS likely results from large contributions from x-ray induced electron stimulated desorption of ions, and does not necessarily indicate that the electronic structure of the bulk liquid and liquid surface are identical.},
doi = {},
journal = {Journal of Physics: Condensed Matter},
number = 20,
volume = 20,
place = {United States},
year = {Sat Feb 16 00:00:00 EST 2008},
month = {Sat Feb 16 00:00:00 EST 2008}
}