Note to users. If you're seeing this message, it means that your browser cannot find this page's style/presentation instructions -- or possibly that you are using a browser that does not support current Web standards. Find out more about why this message is appearing, and what you can do to make your experience of our site the best it can be.

Originally published in Science Express on 1 April 2004
Science 14 May 2004:
Vol. 304. no. 5673, pp. 995 - 999
DOI: 10.1126/science.1096205
Prev | Table of Contents | Next

Reports

The Structure of the First Coordination Shell in Liquid Water

Ph. Wernet,1,2 D. Nordlund,3 U. Bergmann,1 M. Cavalleri,3 M. Odelius,3 H. Ogasawara,1,3 L. Å. Näslund,1,3 T. K. Hirsch,4 L. Ojamäe,5 P. Glatzel,6 L. G. M. Pettersson,3 A. Nilsson1,3*

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 of ordinary hexagonal 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°C 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.

1 Stanford Synchrotron Radiation Laboratory, Post Office Box 20450, Stanford, CA 94309, USA.
2 BESSY, Albert-Einstein-Strasse 15, D-12489 Berlin, Germany.
3 FYSIKUM, Stockholm University, AlbaNova, S-10691 Stockholm, Sweden.
4 Department of Physical Chemistry, Stockholm University, S-10691 Stockholm, Sweden.
5 Department of Chemistry, Linköping University, S-58183 Linköping, Sweden.
6 Department of Inorganic Chemistry and Catalysis, Debye Institute, Utrecht University, Sorbonnelaan 16, 3584 CA Utrecht, Netherlands.

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

Read the Full Text


THIS ARTICLE HAS BEEN CITED BY OTHER ARTICLES:
The inhomogeneous structure of water at ambient conditions.
C. Huang, K. T. Wikfeldt, T. Tokushima, D. Nordlund, Y. Harada, U. Bergmann, M. Niebuhr, T. M. Weiss, Y. Horikawa, M. Leetmaa, et al. (2009)
PNAS 106, 15214-15218
   Abstract »    Full Text »    PDF »
X-ray Raman scattering study of MgSiO3 glass at high pressure: Implication for triclustered MgSiO3 melt in Earth's mantle.
S. K. Lee, J.-F. Lin, Y. Q. Cai, N. Hiraoka, P. J. Eng, T. Okuchi, H.-k. Mao, Y. Meng, M. Y. Hu, P. Chow, et al. (2008)
PNAS 105, 7925-7929
   Abstract »    Full Text »    PDF »
Temperature dependence of the two-dimensional infrared spectrum of liquid H2O.
D. Kraemer, M. L. Cowan, A. Paarmann, N. Huse, E. T. J. Nibbering, T. Elsaesser, and R. J. D. Miller (2008)
PNAS 105, 437-442
   Abstract »    Full Text »    PDF »
Multidimensional Ultrafast Spectroscopy Special Feature: Hydrogen bonding and Raman, IR, and 2D-IR spectroscopy of dilute HOD in liquid D2O.
B. Auer, R. Kumar, J. R. Schmidt, and J. L. Skinner (2007)
PNAS 104, 14215-14220
   Abstract »    Full Text »    PDF »
Epoxide-Opening Cascades Promoted by Water.
I. Vilotijevic and T. F. Jamison (2007)
Science 317, 1189-1192
   Abstract »    Full Text »    PDF »
Predictions of the Properties of Water from First Principles.
R. Bukowski, K. Szalewicz, G. C. Groenenboom, and A. van der Avoird (2007)
Science 315, 1249-1252
   Abstract »    Full Text »    PDF »
Tetrahedral structure or chains for liquid water.
T. Head-Gordon and M. E. Johnson (2006)
PNAS 103, 7973-7977
   Abstract »    Full Text »    PDF »
Scientific Advances Made Possible by User Facilities.
G. E. Brown Jr., G. Calas, and R. J. Hemley (2006)
Elements 2, 23-30
   Abstract »    Full Text »    PDF »
Neutron Scattering and Diffraction Studies of Fluids and Fluid-Solid Interactions.
D. R. Cole, K. W. Herwig, E. Mamontov, and J. Z. Larese (2006)
Reviews in Mineralogy and Geochemistry 63, 313-362
   Full Text »    PDF »
Unified description of temperature-dependent hydrogen-bond rearrangements in liquid water.
J. D. Smith, C. D. Cappa, K. R. Wilson, R. C. Cohen, P. L. Geissler, and R. J. Saykally (2005)
PNAS 102, 14171-14174
   Abstract »    Full Text »    PDF »
Comment on "Energetics of Hydrogen Bond Network Rearrangements in Liquid Water".
A. Nilsson, Ph. Wernet, D. Nordlund, U. Bergmann, M. Cavalleri, M. Odelius, H. Ogasawara, L.-A. Naslund, T. K. Hirsch, L. Ojamae, et al. (2005)
Science 308, 793a
   Full Text »    PDF »
Response to Comment on "Energetics of Hydrogen Bond Network Rearrangements in Liquid Water".
J. D. Smith, C. D. Cappa, B. M. Messer, R. C. Cohen, and R. J. Saykally (2005)
Science 308, 793b
   Full Text »    PDF »
Energetics of Hydrogen Bond Network Rearrangements in Liquid Water.
J. D. Smith, C. D. Cappa, K. R. Wilson, B. M. Messer, R. C. Cohen, and R. J. Saykally (2004)
Science 306, 851-853
   Abstract »    Full Text »    PDF »


To Advertise     Find Products

Science. ISSN 0036-8075 (print), 1095-9203 (online)