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Register a new userQ-dependent Collective Relaxation Dynamics of Glass-Forming Liquid Ca0.4K0.6(NO3)1.4 Investigated by Wide-Angle Neutron Spin-Echo
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Employing wide-angle neutron spin echo spectroscopy, we measured the Q-dependent coherent intermediate scattering function of the prototypical ionic glass former Ca0.4K0.6(NO3)1.4, in the equilibrium and supercooled liquid states beyond the hydrodynamic regime. The data reveal a clear two-step relaxation: an exponential fast process, and a stretched exponential slow alpha process. de Gennes narrowing is observed in all characteristic variables of the alpha process: the relaxation time, amplitude, and stretching exponent. At all length scales probed, the relative amplitude of the alpha-relaxation decreases with increasing temperature and levels off in the normal liquid state. The temperature dependence of the stretching exponent and the relaxation time at different Qs indicate that modifications of the relaxation mechanisms at the local length scales, manifested as temperature independent dynamic heterogeneity and smaller deviations from Arrhenius behavior, have occurred even above the alpha-beta (Johari-Goldstein) bifurcation temperature.
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We present the first inelastic neutron scattering study of the short wavelength dynamics in a phospholipid bilayer. We show that inelastic neutron scattering using a triple-axis spectrometer at the high flux reactor of the ILL yields the necessary resolution and signal to determine the dynamics of model membranes. The results can quantitatively be compared to recent Molecular Dynamics simulations. Reflectivity, in-plane correlations and the corresponding dynamics can be measured simultaneously to gain a maximum amount of information. With this method, dispersion relations can be measured with a high energy resolution. Structure and dynamics in phospholipid bilayers, and the relation between them, can be studied on a molecular length scale.
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On approaching the glass transition, the microscopic kinetic unit spends increasing time rattling in the cage of the first neighbours whereas its average escape time, the structural relaxation time $tau_alpha$, increases from a few picoseconds up to thousands of seconds. A thorough study of the correlation between $tau_alpha$ and the rattling amplitude, expressed by the Debye-Waller factor (DW), was carried out. Molecular-dynamics (MD) simulations of both a model polymer system and a binary mixture were performed by varying the temperature, the density $rho$, the potential and the polymer length to consider the structural relaxation as well as both the rotational and the translation diffusion. The simulations evidence the scaling between the $tau_alpha$ and the Debye-Waller factor. An analytic model of the master curve is developed in terms of two characteristic length scales pertaining to the distance to be covered by the kinetic unit to reach a transition state. The model does not imply $tau_alpha$ divergences. The comparison with the experiments supports the numerical evidence over a range of relaxation times as wide as about eighteen orders of magnitude. A comparison with other scaling and correlation procedures is presented. The study suggests that the equilibrium and the moderately supercooled states of the glassformers possess key information on the huge slowing-down of their relaxation close to the glass transition. The latter, according to the present simulations, exhibits features consistent with the Lindemann melting criterion and the free-volume model.
We have studied the collective short wavelength dynamics in deuterated DMPC bilayers by inelastic neutron scattering. The corresponding dispersion relation $hbaromega$(Q) is presented for the gel and fluid phase of this model system. The temperature dependence of the inelastic excitations indicates a phase coexistence between the two phases over a broad range and leads to a different assignment of excitations than that reported in a preceding inelastic x-ray scattering study [Phys. Rev. Lett. {bf 86}, 740 (2001)]. As a consequence, we find that the minimum in the dispersion relation is actually deeper in the gel than in the fluid phase. Finally, we can clearly identify an additional non-dispersive (optical) mode predicted by Molecular Dynamics (MD) simulations [Phys. Rev. Lett. {bf 87}, 238101 (2001)].
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