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.
Article Details
Journal Info
The Journal of Chemical Physics
American Institute of Physics
Authors (25)
Tomoki Fujita
Department of Chemistry, Aarhus University 1 , 8000 Aarhus,
Yanwen Sun
Linac Coherent Light Source, SLAC National Accelerator Laboratory
Haoyuan Li
Icahn Genomics Institute, Precision Immunology Institute, Department of Immunology and Immunotherapy, Department of Oncological Sciences, Tisch Cancer Institute, Biomedical Engineering and Imaging Institute, Friedman Brain Institute
Thies J. Albert
Faculty of Physics and Center for Nanointegration Duisburg-Essen (CENIDE), University of Duisburg-Essen 4 , Lotharstrasse 1, 47048 Duisburg,
Sanghoon Song
Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States
Takahiro Sato
Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, United States
Jens Moesgaard
Department of Chemistry, Aarhus University 1 , 8000 Aarhus,
Antoine Cornet
Institut Néel, CNRS 5 , 38042 Grenoble,
Peihao Sun
Ying Chen
Mianzhen Mo
Linac Coherent Light Source, SLAC National Accelerator Laboratory 2 , Menlo Park, California 94025,
Narges Amini
Department of Chemistry, Aarhus University 1 , 8000 Aarhus,
Fan Yang
Pierre Lucas
Vincent Esposito
Linac Coherent Light Source, SLAC National Accelerator Laboratory 2 , Menlo Park, California 94025,
Joan Vila-Comamala
Nan Wang
Talgat Mamyrbayev
Paul Scherrer Institute
Christian David
Paul Scherrer Institute
Jerome Hastings
Beatrice Ruta
Institut Néel, CNRS 5 , 38042 Grenoble,
Paul Fuoss
Linac Coherent Light Source, SLAC National Accelerator Laboratory 2 , Menlo Park, California 94025,
Klaus Sokolowski-Tinten
Faculty of Physics and Center for Nanointegration Duisburg-Essen (CENIDE), University of Duisburg-Essen 4 , Lotharstrasse 1, 47048 Duisburg,
Diling Zhu
Linac Coherent Light Source, SLAC National Accelerator Laboratory
Shuai Wei