CSPEC: The cold chopper spectrometer of the ESS, a detailed overview prior to commissioning.

CSPEC is the cold chopper spectrometer of the European Spallation Source (ESS) and will come online with the ESS beam on the target. CSPEC will be the first cold chopper spectrometer on a long pulsed spallation source, which provides great opportunities in terms of signal to noise and novel measuring schemes. We provide a detailed overview of the instrument, scientific design considerations, and engineering requirements.

Crowding effect on helix-coil transition: beyond entropic stabilization.

We report circular dichroism measurements on the helix-coil transition of poly(L-glutamic acid) in solution with polyethylene glycol (PEG) as a crowding agent. The PEG solutions have been characterized by small angle neutron scattering and are well described by the picture of a network of mesh size ξ, usual for semi-dilute chains in good solvent. We show that the increase of PEG concentration stabilizes the helices and increases the transition temperature. But more unexpectedly, we also notice that the increase of concentration of crowding agent reduces the mean helix extent at the transition, or in other words reduces its cooperativity. This result cannot be taken into account for by an entropic stabilization mechanism. Comparing the mean length of helices at the transition and the mesh size of the PEG network, our results strongly suggest two regimes: helices shorter or longer than the mesh size.

Compression of random coils due to macromolecular crowding: scaling effects.

The addition of a macromolecular crowding agent to a dilute solution of polymer exerts a compressive force that tends to reduce the size of the chain. We study here the effect of changing the size ratio between the random coil and the crowding agent. The compression occurs at lower crowding agent concentration, Φ when polymer molecular weight increases. The Flory exponent ν(Φ) decreases from ν(0)≃0.48 in water down to 0.3 with macromolecular crowding. The effective polymer-polymer interactions change from repulsive to strongly attractive inducing aggregation of the chains. This effect changes drastically for larger polymer sizes, being much more pronounced at high molecular weights.

Compression of random coils due to macromolecular crowding.

The conformation of a linear polymer chain is studied as a function of the concentration of a macromolecular crowding agent by neutron scattering. Excluded volume to random coil due to macromolecular crowding in cells is predicted to exert a compressive force that will tend to reduce its size. It is shown that when reducing free volume due to macromolecular crowding, we observe a compression of the polymer chain with a reduction in its radius of gyration of up to approximately 30% and that the effective chain-chain interactions are strongly modified.

Signature of low-dimensional diffusion in complex systems.

We present a clear signature of the dimensionality of water diffusion in a powder sample of a synthetic hectorite (a model clay), by analyzing the corresponding neutron scattering functions. The data follow the theoretical predictions for a powder-averaged two-dimensional diffusion, with a two-dimensional diffusion coefficient of 0.75 x 10(-9) m2 s(-1). Neutron scattering data of bulk water are used as a reference, representing motion in three dimensions. The approach is based on analyzing the scattered intensity at zero energy transfers, along with the broadening of the scattering functions, collected at a wide range of energy resolutions. The mathematical relationship between these two quantities follows, for a given shape of the resolution function, a universal master curve, independent of the diffusion coefficient, but strongly dependent on the dimensionality of the motion, which can thus be determined with clarity.

Dynamics of water in a molecular sieve by quasielastic neutron scattering.

We have investigated the dynamics of water confined in a molecular sieve, with a cylindrical pore diameter of 10 A, by means of quasielastic neutron scattering (QENS). Both the incoherent and coherent intermediate scattering functions I(Q,t) were determined by time-of-flight QENS and the neutron spin-echo technique, respectively. The results show that I(Q,t) is considerably more stretched in time with a slightly larger average relaxation time in the case of coherent scattering. From the Q dependence of I(Q,t) it is clear that the observed dynamics is almost of an ordinary translational nature. A comparison with previous dielectric measurements suggests a possible merging of the alpha and beta relaxations of the confined water at T=185 K, although the alpha relaxation cannot be directly observed at lower temperatures due to the severe confinement. The present results are discussed in relation to previous results for water confined in a Na-vermiculite clay, where the average relaxation time from spin-echo measurements was found to be slower than in the present system (particularly at low temperatures).

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.

Experimental evidence for fast heterogeneous collective structural relaxation in a supercooled liquid near the glass transition

We have extended the exploration of microscopic dynamics of supercooled liquids to small wave numbers Q corresponding to the scale of intermediate range order, by developing a new experimental approach for precise data correction for multiple scattering noise in inelastic coherent neutron scattering. Our results in supercooled Ca0.4K0.6(NO3)(1.4) reveal the first direct experimental evidence, after a decade of controversy, that the so-called picosecond process around the glass transition corresponds to a predicted first, faster stage of the structural relaxation. In addition, they show that this process takes the spatial form of fast heterogeneous collective flow of correlated groups of atoms.