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Title: Microscopic signatures of yielding in concentrated nanoemulsions under large-amplitude oscillatory shear

Abstract

Here, we report x-ray photon correlation spectroscopy (XPCS) experiments on a series of concentrated oil-in-water nanoemulsions with varying droplet volume fraction subjected to in situ steady-state large-amplitude oscillatory shear (LAOS). The shear strain causes periodic echoes in the x-ray speckle patterns that lead to peaks in the intensity autocorrelation function. Above an onset strain amplitude that depends on nanoemulsion concentration, the peaks become attenuated, signaling spatially heterogeneous, shear-induced droplet dynamics. These dynamics include irreversible re- arrangements among the droplets that occur in some regions of the nanoemulsions during a given shear cycle and residual strain-like displacements in those regions that do not re-arrange. The wave-vector dependence of the peak attenuation indicates a power-law distribution in the size of regions undergoing shear-induced rearrangement that is similar to that observed previously in LAOS-XPCS measurements on concentrated nanocolloidal gels. The values of the onset strains for re-arrangement correlate with the concentration-dependent macroscopic yielding behavior of the nanoemulsions. Specically, they occur below the strains at which the nanoemulsions become effectively uidized and, except for the lowest concentration nanoemulsion in the study, signicantly above the threshold strain for nonlinear rheological response.

Authors:
 [1];  [2];  [3];  [3];  [4];  [1];  [2]
  1. Univ. of Ottawa, Ottawa, ON (Canada)
  2. Johns Hopkins Univ., Baltimore, MD (United States)
  3. Univ. of California-Los Angeles, Los Angeles, CA (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); Natural Sciences and Engineering Research Council of Canada (NSERC); University of California, Los Angeles (UCLA); USDOE
OSTI Identifier:
1489762
Alternate Identifier(s):
OSTI ID: 1469257
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 9; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Rogers, Michael C., Chen, Kui, Pagenkopp, Matthew J., Mason, Thomas G., Narayanan, Suresh, Harden, James L., and Leheny, Robert L. Microscopic signatures of yielding in concentrated nanoemulsions under large-amplitude oscillatory shear. United States: N. p., 2018. Web. doi:10.1103/PhysRevMaterials.2.095601.
Rogers, Michael C., Chen, Kui, Pagenkopp, Matthew J., Mason, Thomas G., Narayanan, Suresh, Harden, James L., & Leheny, Robert L. Microscopic signatures of yielding in concentrated nanoemulsions under large-amplitude oscillatory shear. United States. https://doi.org/10.1103/PhysRevMaterials.2.095601
Rogers, Michael C., Chen, Kui, Pagenkopp, Matthew J., Mason, Thomas G., Narayanan, Suresh, Harden, James L., and Leheny, Robert L. Mon . "Microscopic signatures of yielding in concentrated nanoemulsions under large-amplitude oscillatory shear". United States. https://doi.org/10.1103/PhysRevMaterials.2.095601. https://www.osti.gov/servlets/purl/1489762.
@article{osti_1489762,
title = {Microscopic signatures of yielding in concentrated nanoemulsions under large-amplitude oscillatory shear},
author = {Rogers, Michael C. and Chen, Kui and Pagenkopp, Matthew J. and Mason, Thomas G. and Narayanan, Suresh and Harden, James L. and Leheny, Robert L.},
abstractNote = {Here, we report x-ray photon correlation spectroscopy (XPCS) experiments on a series of concentrated oil-in-water nanoemulsions with varying droplet volume fraction subjected to in situ steady-state large-amplitude oscillatory shear (LAOS). The shear strain causes periodic echoes in the x-ray speckle patterns that lead to peaks in the intensity autocorrelation function. Above an onset strain amplitude that depends on nanoemulsion concentration, the peaks become attenuated, signaling spatially heterogeneous, shear-induced droplet dynamics. These dynamics include irreversible re- arrangements among the droplets that occur in some regions of the nanoemulsions during a given shear cycle and residual strain-like displacements in those regions that do not re-arrange. The wave-vector dependence of the peak attenuation indicates a power-law distribution in the size of regions undergoing shear-induced rearrangement that is similar to that observed previously in LAOS-XPCS measurements on concentrated nanocolloidal gels. The values of the onset strains for re-arrangement correlate with the concentration-dependent macroscopic yielding behavior of the nanoemulsions. Specically, they occur below the strains at which the nanoemulsions become effectively uidized and, except for the lowest concentration nanoemulsion in the study, signicantly above the threshold strain for nonlinear rheological response.},
doi = {10.1103/PhysRevMaterials.2.095601},
journal = {Physical Review Materials},
number = 9,
volume = 2,
place = {United States},
year = {Mon Sep 10 00:00:00 EDT 2018},
month = {Mon Sep 10 00:00:00 EDT 2018}
}

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Cited by: 21 works
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