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Dynamics of supercooled confined water measured by deep inelastic neutron scattering

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Abstract

In this paper, we present the results of deep inelastic neutron scattering (DINS) measurements on supercooled water confined within the pores (average pore diameter ~ 20 Å) of a disordered hydrophilic silica matrix obtained through hydrolysis and polycondensation of the alkoxide precursor Tetra-Methyl-Ortho-Silicate via the sol-gel method. Experiments were performed at two temperatures (250 K and 210 K, i.e., before and after the putative liquid–liquid transition of supercooled confined water) on a “wet” sample with hydration h ~ 40% w/w, which is high enough to have water-filled pores but low enough to avoid water crystallization. A virtually “dry” sample at h ~ 7% was also investigated to measure the contribution of the silica matrix to the neutron scattering signal. As is well known, DINS measurements allow the determination of the mean kinetic energy and the momentum distribution of the hydrogen atoms in the system and therefore, allow researchers to probe the local structure of supercooled confined water. The main result obtained is that at 210 K the hydrogen mean kinetic energy is equal or even slightly higher than at 250 K. This is at odds with the predictions of a semiempirical harmonic model recently proposed to describe the temperature dependence of the kinetic energy of hydrogen in water. This is a new and very interesting result, which suggests that at 210 K, the water hydrogens experience a stiffer intermolecular potential than at 250 K. This is in agreement with the liquid–liquid transition hypothesis.

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Acknowledgements

V. D. M. and A. C. thank the members of the Molecular Biophysics and Nanotechnology group at the University of Palermo, Italy, for useful discussions and their indirect financial support. Financial support from Italian CNR (Dipartimento di Scienze Fisiche e Tecnologie della Materia) is also gratefully acknowledged; in fact, this work was supported under the CNR-STFC Agreement (2014–2020) concerning collaboration in scientific research at the ISIS pulsed neutron and muon source.

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Authors and Affiliations

  1. Dipartimento di Fisica e Chimica, Università di Palermo, Viale delle Scienze Ed. 18, 90128, Palermo, Italy

    Vincenzo De Michele & Antonio Cupane

  2. ISIS Facility, Rutherford Appleton Laboratory, Chilton, Didcot, Oxfordshire, OX11 0QX, UK

    Giovanni Romanelli

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  1. Vincenzo De Michele
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  2. Giovanni Romanelli
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  3. Antonio Cupane
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Correspondence to Antonio Cupane.

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De Michele, V., Romanelli, G. & Cupane, A. Dynamics of supercooled confined water measured by deep inelastic neutron scattering. Front. Phys. 13, 138205 (2018). https://doi.org/10.1007/s11467-017-0699-1

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