Investigation of the yielding transition in concentrated colloidal systems via rheo-XPCS

Author:

Donley Gavin J.123,Narayanan Suresh4,Wade Matthew A.1ORCID,Park Jun Dong5,Leheny Robert L.6ORCID,Harden James L.7,Rogers Simon A.1ORCID

Affiliation:

1. Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana-Champaign, Urbana, IL 61801

2. Department of Physics & Institute for Soft Matter Synthesis and Metrology, Georgetown University, Washington, DC 20057

3. Infrastructure Materials Group, Materials and Structural Systems Division, Engineering Laboratory, National Institute of Standards and Technology, Gaithersburg, MD 20899

4. X-ray Science Division, Argonne National Laboratory, Lemont, IL 60439

5. Department of Chemical Engineering, Sookmyung Women’s University, Seoul 04310, Korea

6. Department of Physics and Astronomy, Johns Hopkins University, Baltimore, MD 21218

7. Department of Physics, University of Ottawa, Ottawa, ON K1N 6N5, Canada

Abstract

We probe the microstructural yielding dynamics of a concentrated colloidal system by performing creep/recovery tests with simultaneous collection of coherent scattering data via X-ray Photon Correlation Spectroscopy (XPCS). This combination of rheology and scattering allows for time-resolved observations of the microstructural dynamics as yielding occurs, which can be linked back to the applied rheological deformation to form structure–property relations. Under sufficiently small applied creep stresses, examination of the correlation in the flow direction reveals that the scattering response recorrelates with its predeformed state, indicating nearly complete microstructural recovery, and the dynamics of the system under these conditions slows considerably. Conversely, larger creep stresses increase the speed of the dynamics under both applied creep and recovery. The data show a strong connection between the microstructural dynamics and the acquisition of unrecoverable strain. By comparing this relationship to that predicted from homogeneous, affine shearing, we find that the yielding transition in concentrated colloidal systems is highly heterogeneous on the microstructural level.

Funder

National Science Foundation

DOE | NNSA | Laboratory Directed Research and Development

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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