Issue 20, 2009
From the journal:

Physical Chemistry Chemical Physics

Probing the hydrogen-bond network of watervia time-resolved soft X-ray spectroscopy

Nils Huse,†*a   Haidan Wen,†b   Dennis Nordlund,c   Erzsi Szilagyi,bd   Dan Daranciang,bd   Timothy A. Miller,be   Anders Nilsson,cf   Robert W. Schoenleinag  and  Aaron M. Lindenbergbe  

* Corresponding authors

a Chemical Sciences Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, USA
E-mail: nhuse@lbl.gov

b PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, USA

c Stanford Synchrotron Radiation Laboratory, P.O.B. 20450, Stanford, USA

d Department of Chemistry, Stanford University, Stanford, USA

e Department of Materials Science and Engineering, Stanford University, Stanford, USA

f FYSIKUM, Stockholm University, Alba Nova, Stockholm, Sweden

g Materials Sciences Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, USA

Abstract

We report time-resolved studies of hydrogen bonding in liquid H2O, in response to direct excitation of the O–H stretch mode at 3 μm, probed via soft X-ray absorption spectroscopy at the oxygen K-edge. This approach employs a newly developed nanofluidic cell for transient soft X-ray spectroscopy in the liquid phase. Distinct changes in the near-edge spectral region (XANES) are observed, and are indicative of a transient temperature rise of 10 K following transient laser excitation and rapid thermalization of vibrational energy. The rapid heating occurs at constant volume and the associated increase in internal pressure, estimated to be 8 MPa, is manifested by distinct spectral changes that differ from those induced by temperature alone. We conclude that the near-edge spectral shape of the oxygen K-edge is a sensitive probe of internal pressure, opening new possibilities for testing the validity of water models and providing new insight into the nature of hydrogen bonding in water.

Graphical abstract: Probing the hydrogen-bond network of water via time-resolved soft X-ray spectroscopy

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Article information

DOI
https://doi.org/10.1039/B822210J
Article type
Paper
Submitted
10 Dec 2008
Accepted
05 Feb 2009
First published
10 Mar 2009

Phys. Chem. Chem. Phys., 2009,11, 3951-3957

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Probing the hydrogen-bond network of water via time-resolved soft X-ray spectroscopy

N. Huse, H. Wen, D. Nordlund, E. Szilagyi, D. Daranciang, T. A. Miller, A. Nilsson, R. W. Schoenlein and A. M. Lindenberg, Phys. Chem. Chem. Phys., 2009, 11, 3951 DOI: 10.1039/B822210J

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