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Published Online April 1, 2004
Science DOI: 10.1126/science.1096205

Reports

Submitted on January 29, 2004
Accepted on March 25, 2004

The Structure of the First Coordination Shell in Liquid Water

Ph. Wernet 1, D. Nordlund 2, U. Bergmann 3, M. Cavalleri 2, M. Odelius 2, H. Ogasawara 4, L. Å. Näslund 4, T. K. Hirsch 5, L. Ojamäe 6, P. Glatzel 7, L. G. M. Pettersson 2, A. Nilsson 4*

1 Stanford Synchrotron Radiation Laboratory, Post Office Box 20450, Stanford, CA 94309, USA; Present address: BESSY, Albert-Einstein-Strasse 15, D-12489 Berlin, Germany.
2 FYSIKUM, Stockholm University, AlbaNova, S-106 91 Stockholm, Sweden.
3 Stanford Synchrotron Radiation Laboratory, Post Office Box 20450, Stanford, CA 94309, USA.
4 Stanford Synchrotron Radiation Laboratory, Post Office Box 20450, Stanford, CA 94309, USA; FYSIKUM, Stockholm University, AlbaNova, S-106 91 Stockholm, Sweden.
5 Department of Physical Chemistry, Stockholm University, S-106 91 Stockholm, Sweden.
6 Department of Chemistry, Linköping University, S-58183 Linköping, Sweden.
7 Department of Inorganic Chemistry and Catalysis, Debye Institute, Utrecht University, 3584 CA Utrecht, Netherlands.

* To whom correspondence should be addressed.
A. Nilsson , E-mail: nilsson{at}slac.stanford.edu

X-ray absorption spectroscopy and x-ray Raman scattering were used to probe the molecular arrangement in the first coordination shell of liquid water. The local structure is characterized by comparison with bulk and surface ice Ih and with calculated spectra. Most molecules in liquid water are in two-hydrogen-bonded configurations with one strong donor and one strong acceptor hydrogen bond in contrast to the four-hydrogen-bonded tetrahedral structure in ice. Upon heating from 25° to 90°C, 5 to 10% of the molecules change from tetrahedral environments to two-hydrogen-bonded configurations. Our findings are consistent with neutron and x-ray diffraction data, and combining the results sets a strong limit for possible local structure distributions in liquid water. Serious discrepancies with structures based on current molecular dynamics simulations are observed.


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