The structural differences between the compositionally related Pt-P-and Pd-P-based bulk glass-forming liquids are investigated in synchrotron X-ray scattering experiments. Although Pt and Pd are considered to be topologically equivalent in structural models, we show that drastic changes in the total structure factor and in the reduced pair distribution function are observed upon gradual substitution. These variations indicate the existence of significant structural differences on the short-(SRO) and medium-range order (MRO) length scale. The structural data suggest that the distribution of the dominant polyhedra and the distribution of their connection schemes gradually change from Pt-P-to Pd-P-based alloys, which is likely connected to the different sensitivities to annealing or cooling rate induced embrittlement. The evolution of the total structure factor and the reduced pair distribution function with increasing temperature indicate the (partial) dissolution of both, the MRO and the SRO, which reflects the thermodynamic properties of the liquids.
We present a detailed investigation of the wave-vector dependence of collective atomic motion in Au 49 Cu 26.9 Si 16.3 Ag 5.5 Pd 2.3 and Pd 42.5 Cu 27 Ni 9.5 P 21 supercooled liquids close to the glass transition temperature. Using x-ray photon correlation spectroscopy in a previously uncovered spatial range of only a few interatomic distances, we show that the microscopic structural relaxation process mimics the structure and presents a marked slowing down at the main average interparticle distance. This behavior is accompanied by dramatic changes in the shape of the intermediate scattering functions, which suggest the presence of large dynamical heterogeneities at length scales corresponding to a few particle diameters. A ballisticlike mechanism of particle motion seems to govern the structural relaxation of the two systems in the highly viscous phase, likely associated with hopping of caged particles in agreement with theoretical studies.
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