Abstract
HYDROGEN bonds play a crucial role in the behaviour of water1–4; their spatial patterns and fluctuations characterize the structure and dynamics of the liquid5–7. The processes of breaking and making hydrogen bonds in the condensed phase can be probed indirectly by a variety of experimental techniques8, and more quantitative information can be obtained from computer simulations9. In particular, simulations have revealed that on long timescales the relaxation behaviour of hydrogen bonds in liquid water exhibit non-exponential kinetics7,10–13, suggesting that bond making and breaking are not simple processes characterized by well defined rate constants. Here we show that these kinetics can be understood in terms of an interplay between diffusion and hydrogen-bond dynamics. In our model, which can be extended to other hydrogen-bonded liquids, diffusion governs whether a specific pair of water molecules are near neighbours, and hydrogen bonds between such pairs form and persist at random with average lifetimes determined by rate constants for bond making and breaking.
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References
Teixeira, J. J. Physique IV C1, 3, 162–169 (1993).
Eisenberg, D. & Kauzmann, W. The Structure and Properties of Water (Oxford Univ. Press, New York, 1969).
Franks, F. (ed.) Water Science Reviews Vols 1–5 (Cambridge Univ. Press, 1985–90).
Stanley, H. E. & Ostrowzky, N. (eds) Correlations and Connectivity, Geometric Aspects of Physics, Chemistry and Biology (Kluwer Academic, Dordrecht, 1990).
Stillinger, F. H. Adv. chem. Phys. 31, 1–101 (1975).
Stillinger, F. H. Science 209, 451–457 (1980).
Ohmine, I. & Tanaka, H. Chem. Rev. 93, 2545–2566 (1993).
Dore, J. C. & Teixeira, J. (eds) Hydrogen-Bonded Liquids (Kluwer Academic, Dordrecht, 1991).
Ladanyi, B. M. & Skaf, M. S. A. Rev. Chem. 44, 335–368 (1993).
Belch, A. C. & Rice, S. A. J. chem. Phys. 86, 5676–5682 (1987).
Sciortino, F., Poole, P. H., Stanley, H. E. & Havlin, S. Phys. Rev. Lett. 64, 1686–1689 (1990).
Zichi, D. A. & Rossky, P. J. J. chem. Phys. 84, 2814–2822 (1986).
Luzar, A. & Chandler, D. in Hydrogen Bond Networks (eds Bellisent-Funel, M. C. & Dore, J. C.) 239–246 (Kluwer Academic, Dordrecht, 1994).
Chandler, D. Introduction to Modern Statistical Mechanics (Oxford Univ. Press, New York, 1987).
Chandler, D. J. chem. Phys. 68, 2959–2970 (1978).
Berne, B. J. in Multiple Time Scales (eds Brackbill, J. U. & Cohen, B. I.) 419–436 (Academic, New York, 1985).
Saito, S. & Ohmine, I. J. chem. Phys. 102, 3566–3579 (1995).
Ferrario, M., Haughley, M., McDonald, I. R. & Klein, M. L. J. chem. Phys. 93, 5156–5166 (1990).
Luzar, A. & Chandler, D. J. chem. Phys. 98, 8160–8173 (1993).
Soper, A. K. & Phillips, M. G. Chem. Phys. 107, 47–60 (1986).
Teixeira, J., Bellissent-Funel, M.-C., Chen, S. H. & Dianoux, A. J. Phys. Rev. A31, 1913–1917 (1985).
Bratos, S. & Leicknam, J.-C. J. chem. Phys. 103, 4887–4893 (1995).
Berendsen, H. J. C., Postma, J. P. M., van Gusteren, W. F. & Hermans, J. in Intermolecular Forces (ed. Pullman, B.) 331–342 (Reidel, Dordrecht, 1981).
Allan, M. P. & Tildesley, D. J. Computer Simulation of Liquids (Clarendon, Oxford, 1987).
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Luzar, A., Chandler, D. Hydrogen-bond kinetics in liquid water. Nature 379, 55–57 (1996). https://doi.org/10.1038/379055a0
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DOI: https://doi.org/10.1038/379055a0
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