Quasi-elastic neutron scattering has been used to study atomic relaxation processes in high-entropy glass-forming metallic melts with different glass-forming ability (GFA). The momentum transfer dependence of mean relaxation time shows a highly collective atomic transport process in the alloy melts with the highest and lowest GFA. However, a jump diffusion process is the long-range atomic transport process in the intermediate GFA alloy melt. Nevertheless, atomic mobility close to the melting temperature of these alloy melts is quite similar, and the temperature dependence of the diffusion coefficient exhibits a non-Arrhenius behavior. The atomic mobility in these high-entropy melts is much slower than that of the best glass-forming melts at their respective melting temperatures.
The precise nature of complex structural relaxation as well as an explanation for the precipitous growth of relaxation time in cooling glass-forming liquids are essential to the understanding of vitrification of liquids. The dramatic increase of relaxation time is believed to be caused by the growth of one or more correlation lengths, which has received much attention recently. Here, we report a direct link between the growth of a specific local-geometrical-order and an increase of dynamic-length-scale as the atomic dynamics in metallic glass-forming liquids slow down. Although several types of local geometrical-orders are present in these metallic liquids, the growth of icosahedral ordering is found to be directly related to the increase of the dynamic-length-scale. This finding suggests an intriguing scenario that the transient icosahedral connectivity could be the origin of the dynamic-length-scale in metallic glass-forming liquids.
Logarithmic relaxation is a unique relaxation process exhibited by a few molecular liquids and biomolecules. However, the microscopic origin of logarithmic relaxation is still unclear. To understand the origin of this process, we studied two liquids that exhibit logarithmic relaxation in a dissolved state using quasielastic neutron scattering (QENS) and depolarized dynamic light scattering (DDLS). Although the intermolecular potential of the liquids is drastically different in the dissolved state from the bulk liquids, we observed that the logarithmic relaxation still persists. Our results indicate that the intermolecular potential does not play a role in determining the logarithmic relaxation process. The coupling of rotational and translational relaxation processes could be the origin of the logarithmic relaxation process exhibited by the molecular liquids.
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