Reply to “Comment to ‘Dynamics of supercooled confined water measured by deep inelastic neutron scattering’ by Y. Finkelstein and R. Moreh”

We reply to the comment [Front. Phys. 14(5), 53605 (2019)] by Y. Finkelstein and R. Moreh on our article Front. Phys. 13(1), 138205 (2018). We agree with some of their criticisms about our calculation of the temperature effect on the kinetic energy of hydrogen atoms of supercooled confined water; we also agree with their statement that, in view of the current sensitivity of the technique, possible effects of the liquid–liquid water transition are hardly detected with deep inelastic neutron scattering (DINS). However, we disagree with their use of the translational mass ratio of a single water molecule and, in general, with their underestimation of collective effects.     

Dynamics of supercooled confined water measured by deep inelastic neutron scattering

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.     

Dynamics of metal centers monitored by nuclear inelastic scattering

Nuclear inelastic scattering of synchrotron radiation has been used now since 10 years as a tool for vibrational spectroscopy. This method has turned out especially useful in case of large molecules that contain a Mössbauer active metal center. Recent applications to iron–sulfur proteins, to iron(II) spin crossover complexes and to tin-DNA complexes are discussed. Special emphasis is given to the combination of nuclear inelastic scattering and density functional calculations.