TY - JOUR
T1 - High resolution X-ray emission spectroscopy of liquid water
T2 - The observation of two structural motifs
AU - Tokushima, T.
AU - Harada, Y.
AU - Takahashi, O.
AU - Senba, Y.
AU - Ohashi, H.
AU - Pettersson, Lars G.M.
AU - Nilsson, Anders
AU - Shin, S.
PY - 2008/7/30
Y1 - 2008/7/30
N2 - The structure of liquid water is presently under intense debate. We summarize the historical development of the present description of water and the controversy surrounding the X-ray absorption spectroscopy (XAS) study of Wernet et al. [Ph. Wernet et al., Science 304 (2004) 995]. In order to provide further insight into the connection between X-ray spectroscopy and the structure of the hydrogen bonding network, we report new data comprising high resolution oxygen K-edge X-ray emission spectra (XES) of liquid water. We observe two distinct narrow lone-pair derived peaks, assigned, respectively, to tetrahedral and strongly distorted hydrogen-bonded species; the assignment is based on comparison with ice and gas phase spectra, temperature dependent measurements, excitation energy dependence and theoretical simulations. We estimate a 2:1 ratio between distorted and tetrahedral species at room temperature and discuss what this implies in connection to the previous XAS study and in terms of liquid water structure.
AB - The structure of liquid water is presently under intense debate. We summarize the historical development of the present description of water and the controversy surrounding the X-ray absorption spectroscopy (XAS) study of Wernet et al. [Ph. Wernet et al., Science 304 (2004) 995]. In order to provide further insight into the connection between X-ray spectroscopy and the structure of the hydrogen bonding network, we report new data comprising high resolution oxygen K-edge X-ray emission spectra (XES) of liquid water. We observe two distinct narrow lone-pair derived peaks, assigned, respectively, to tetrahedral and strongly distorted hydrogen-bonded species; the assignment is based on comparison with ice and gas phase spectra, temperature dependent measurements, excitation energy dependence and theoretical simulations. We estimate a 2:1 ratio between distorted and tetrahedral species at room temperature and discuss what this implies in connection to the previous XAS study and in terms of liquid water structure.
UR - http://www.scopus.com/inward/record.url?scp=48949116116&partnerID=8YFLogxK
U2 - 10.1016/j.cplett.2008.04.077
DO - 10.1016/j.cplett.2008.04.077
M3 - Article
AN - SCOPUS:48949116116
SN - 0009-2614
VL - 460
SP - 387
EP - 400
JO - Chemical Physics Letters
JF - Chemical Physics Letters
IS - 4-6
ER -