Femtosecond X-ray photon correlation spectroscopy enables direct observations of atomic-scale relaxations of glass forming liquids

Abstract

Glass-forming liquids exhibit structural relaxation behaviors, reflecting underlying atomic rearrangements on a wide range of timescales and playing a crucial role in determining material properties. However, the relaxation processes on the atomic scale are not well-understood due to the experimental difficulties in directly characterizing the evolving correlations of atomic-scale order in disordered systems. Here, we harness the coherence and ultrashort pulse characteristics of an x-ray free electron laser to directly probe atomic-scale ultrafast relaxation dynamics in the model system Ge15Te85. We demonstrate an analysis strategy for determining the intermediate scattering function by extracting the contrast decay of summed scattering patterns from two rapidly successive, nearly identical femtosecond x-ray pulses generated by a split-delay system. The result indicates a full decorrelation of atomic-scale order on the sub-picosecond timescale, supporting the argument for a high-fluidity fragile state of liquid Ge15Te85 above its dynamic crossover temperature. The demonstrated strategy opens an avenue for experimental studies of relaxation dynamics in liquids, glasses, and other highly disordered systems.