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Organisationseinheit der BAM
Highly ordered and highly cooperative water with properties of both solid and liquid states has been observed by means of neutron scattering in hydrophobic one-dimensional channels with van der Waals diameter of 0.78 nm. We have found that in the initial stages of adsorption water molecules occupy niches close to pore walls, followed later by the filling of the central pore area. Intensified by confinement, intermolecular water interactions lead to the formation of well-ordered hydrogen-bonded water chains and to the onset of cooperative vibrations. On the other hand, the same intermolecular interactions lead to two relaxation processes, the faster of which is the spontaneous position exchange between two water molecules placed 3.2-4 A from each other. Self-diffusion in an axial pore direction is the result of those spontaneous random exchanges and is substantially slower than the self-diffusion in bulk water.
The neutron time-of-flight spectrometer NEAT has a long history of successful applications and is best suited to probe dynamic phenomena directly in the large time domain 10(-14) - 10(-10) s and on the length scale ranging from 0.05 to up to about 5 nm. To address user community needs for more powerful instrumental capabilities, a concept of the full upgrade of NEAT has been proposed. The upgrade started in 2010 after a rigorous internal and external selection process and resulted in 300-fold neutron count rate increase compared to NEAT01995. Combined with new instrumental and sample environmental capabilities the upgrade allows NEAT to maintain itself at the best world class level and provide an outstanding experimental tool for a broad range of scientific applications. The advanced features of the new instrument include an integrated guide-chopper system that delivers neutrons with flexible beam properties: either highly homogeneous beam with low divergence suitable for single crystals studies or "hot-spot" neutron distribution serving best small samples. Substantial increase of the detector angle coverage is achieved by using 416 He-3 position sensitive detectors. Placed at 3m from the sample, the detectors cover 20m(2) area and are equipped with modern electronics and DAQ using event recording techniques. The installation of hardware has been completed in June 2016 and on January 23, 2017 NEAT has welcomed its first regular users who took advantage of the high counting rate, broad available range of incoming neutron wavelengths and high flexibility of NEAT. Here we present details of NEAT upgrade, measured instrument characteristics and show first experimental results.
The adsorption of water in one-dimensional channels in porous aluminophosphate material AlPO4-5 has been studied by a combination of gravimetric Analysis techniques, neutron and X-ray diffraction and Neutron spectroscopy. Molecular structure of AlPO4-5 consists of 12-membered rings of alternating, corner-sharing AlO4 and PO4 tetrahedra connected by oxygen bridges into sheets in the (a, b) plane. The sheets are connected by oxygen bridges along the c crystal axis and form onedimensional channels of which the largest, formed by the 12-membered rings, have a van der Waals Diameter of about 8.3 Å. Gradually increasing the amount of adsorbed water we could follow the evolution of the confined water mobility in a systematic way and identify the molecular mechanism of water adsorption. We focused particularly on the range of low and medium relative pressures up to p/p0=0.32, where a Change from a hydrophobic behavior to a steep, capillary condensation like water intake has been observed. At the Initial adsorption stages water occupies positions close to the pore walls causing the contraction of channels in the (a, b) plane and the prolongation of the channels along c axis in AlPO4-5. With the progressing intake water molecules form chains along the main channels. The cooperative interactions between water molecules lead to the onset of phonon-like cooperative modes and, surprisingly, to the increase of diffusive-like motion, which slow down only in the final adsorption stages when AlPO4-5 channels are completely filled.