Dynamics of water studied by coherent and incoherent inelastic neutron scattering

This paper reviews the more recent results obtained on the dynamics of water by neutron scattering and shows that some information can be obtained by this technique at the microscopic level of the hydrogen bond. It also accounts for some very recent results obtained with the hydrated protein C-phycocyanin.

Incoherent quasi-elastic and inelastic neutron scattering by water has been performed in a temperature range extending to the supercooled state. The analysis of the quasi-elastic spectrum separates two main components and gives two characteristic times, one of them being related to the hydrogen-bond lifetime. The inelastic spectra extend until 600 meV, i.e. covering the intramolecular vibration region, showing for the first time the stretching band.

Collective excitations propagating at 3310 m s⁻¹ have been observed by coherent inelastic neutron scattering. This result was predicted by previous computer molecular dynamics simulations of water. The data are interpreted as a manifestation of short wavelength collective modes propagating within patches of highly bonded water molecules, and distinct from the ordinary sound wave.     

Latex Fractionation by Sedimentation and Colloidal Crystallization: The Case of Poly(styrene-co-acrylamide)

Poly(styrene-co-acrylamide) (PS-AAM) latex was prepared, fractionated by sedimentation under gravity, and characterized by PCS, infrared spectra, secondary and backscattered electron imaging in the scanning electron microscope, and electron spectroscopy imaging in an analytical transmission electron microscope. Three latex fractions were obtained. The lower fraction was opalescent and its particles were the more uniform, concerning size, chemical composition, and topochemical features. This lower fraction was still further fractionated by zonal centrifugation in a density gradient, yielding two fractions with similar macrocrystal-forming abilities but different sizes and chemical compositions. These results confirm those previously obtained for the PS-HEMA latex. Copyright 2000 Academic Press.     

Experimental observation of the alpha relaxation in supercooled water

Intermediate scattering functions for density fluctuation in D2O contained in pores of a Vycor glass have been measured using an improved neutron spin-echo spectrometer at two supercooled temperatures. The measurements cover the time range from 1 to 2300 ps with the Q range spanning the first diffraction peak of water. The time correlation functions can be fitted to a stretched exponential relaxation function with a Q-dependent amplitude. Both the stretch exponent and the relaxation time peak approximately at the Q value corresponding to the first diffraction peak, confirming the validity of the mode coupling idea in supercooled water.     

Structure of supercritical water

This review paper gives the more up to date information on the structure of supercritical water, at different thermodynamic states, for densities ranging from 0.2 to 0.7 g.cm⁻³, studied by neutron scattering. The experimental partial pair correlation functions g_OH(r), G_HH(r) and g_OO(r) are compared with the results of molecular dynamics simulations using the (SPCE) model potential for water. The results confirm that hydrogen bonding is still present in dense supercritical water and are in good agreement with data obtained by NMR and Raman spectroscopies.     

Neutron diffraction studies of the structure of water at ambient temperatures,revisited [a review of past developments and current problems]

Neutron diffraction techniques used in the study of the structural characteristics of liquid water under ambient conditions are reviewed, showing the way that developments in the experimental and analytic procedures have led to improvements in the extracted results. The three partial pair correlation functions (OH, HH and OO) can be isolated from a set of diffraction measurements with varying hydrogen/deuterium isotopic composition. Although isotopic substitution is used routinely in many other investigations there are particular difficulties with hydrogenous systems due to the high incoherent scattering from hydrogen and the possibility that the H/D substitution is not a true isomorphic replacement. These features are discussed in some detail to analyse the systematic errors and the precision of the final results. An additional aspect of the comparison of data taken by different groups concerns the use of either reactor or pulsed neutron methods. Studies using the Orphee reactor with an over-determined set of five datasets are considered in detail, using analytic correction procedures based on the Powles formalism. Various consistency checks are applied to the data such that smoothing or iteration routines are not required. Two independent sets of the OD and DD pair correlation functions are obtained and are compared with the latest results from Soper et al. The small discrepancies between the various datasets are discussed in terms of propagating systematic errors and also possible variations from H/D equivalence. The relevance of the new results for the interpretation and modelling of ambient water structure are presented and the review ends with a brief comment on likely future developments that incorporate additional experimental information.     

Diffusional and vibrational dynamics of ZnCl2 aqueous solutions by inelastic neutron scattering

We have studied saturated solutions of ZnCl₂ (and NiCl₂) in D₂O by time-of-flight quasi-elastic and inelastic neutron scattering spectroscopy. Spectra were taken at room temperature as a function of transferred momentum. We find that ionic diffusion in these solutions is best described by a crystal vacancy diffusion model. We also find evidence of collective excitations in the region of ～ 20 meV.