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Title: Nanoscale Critical Phenomena in a Complex Fluid Studied by X-ray Photon Correlation Spectroscopy.

Abstract

The advent of high-speed x-ray photon correlation spectroscopy now allows the study of critical phenomena in fluids to much smaller length scales and over a wider range of temperatures than is possible with dynamic light scattering. We present an x-ray photon correlation spectroscopy study of critical fluctuation dynamics in a complex fluid typical of those used in liquid-liquid extraction (LLE) of ions,dodecane-DMDBTDMA with extracted aqueous Ce(NO3)3. We observe good agreement with both staticand dynamic scaling without the need for significant noncritical background corrections. Critical exponents agree with 3D Ising values, and the fluctuation dynamics are described by simple exponential relaxation.The form of the dynamic master curve deviates somewhat from the Kawasaki result, with a more abrupt transition between the critical and noncritical asymptotic behavior. The concepts of critical phenomena thus provide a quantitative framework for understanding the structure and dynamics of LLE systems and a path forward to new LLE processes.

Authors:
 [1];  [1];  [2];  [1];  [1];  [1];  [1];  [3];  [4];  [4];  [1];  [1];  [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Northern Illinois Univ., DeKalb, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States) ; Univ. of Illinois, Chicago, IL (United States)
  4. AGH - Univ. of Science and Technology, Krakow (Poland)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1661857
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 125; Journal Issue: 12
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
Critical exponents; Critical phenomena; Liquids; X-ray photon correlation spectroscopy

Citation Formats

Sheyfer, D., Zhang, Q., Lal, J., Loeffler, T., Dufresne, E. M., Sandy, A. R., Narayanan, S., Sankaranarayanan, S. K.R.S., Szczygiel, R., Maj, P., Soderholm, L., Antonio, M. R., and Stephenson, G. B. Nanoscale Critical Phenomena in a Complex Fluid Studied by X-ray Photon Correlation Spectroscopy.. United States: N. p., 2020. Web. doi:10.1103/PhysRevLett.125.125504.
Sheyfer, D., Zhang, Q., Lal, J., Loeffler, T., Dufresne, E. M., Sandy, A. R., Narayanan, S., Sankaranarayanan, S. K.R.S., Szczygiel, R., Maj, P., Soderholm, L., Antonio, M. R., & Stephenson, G. B. Nanoscale Critical Phenomena in a Complex Fluid Studied by X-ray Photon Correlation Spectroscopy.. United States. doi:10.1103/PhysRevLett.125.125504.
Sheyfer, D., Zhang, Q., Lal, J., Loeffler, T., Dufresne, E. M., Sandy, A. R., Narayanan, S., Sankaranarayanan, S. K.R.S., Szczygiel, R., Maj, P., Soderholm, L., Antonio, M. R., and Stephenson, G. B. Fri . "Nanoscale Critical Phenomena in a Complex Fluid Studied by X-ray Photon Correlation Spectroscopy.". United States. doi:10.1103/PhysRevLett.125.125504.
@article{osti_1661857,
title = {Nanoscale Critical Phenomena in a Complex Fluid Studied by X-ray Photon Correlation Spectroscopy.},
author = {Sheyfer, D. and Zhang, Q. and Lal, J. and Loeffler, T. and Dufresne, E. M. and Sandy, A. R. and Narayanan, S. and Sankaranarayanan, S. K.R.S. and Szczygiel, R. and Maj, P. and Soderholm, L. and Antonio, M. R. and Stephenson, G. B.},
abstractNote = {The advent of high-speed x-ray photon correlation spectroscopy now allows the study of critical phenomena in fluids to much smaller length scales and over a wider range of temperatures than is possible with dynamic light scattering. We present an x-ray photon correlation spectroscopy study of critical fluctuation dynamics in a complex fluid typical of those used in liquid-liquid extraction (LLE) of ions,dodecane-DMDBTDMA with extracted aqueous Ce(NO3)3. We observe good agreement with both staticand dynamic scaling without the need for significant noncritical background corrections. Critical exponents agree with 3D Ising values, and the fluctuation dynamics are described by simple exponential relaxation.The form of the dynamic master curve deviates somewhat from the Kawasaki result, with a more abrupt transition between the critical and noncritical asymptotic behavior. The concepts of critical phenomena thus provide a quantitative framework for understanding the structure and dynamics of LLE systems and a path forward to new LLE processes.},
doi = {10.1103/PhysRevLett.125.125504},
journal = {Physical Review Letters},
number = 12,
volume = 125,
place = {United States},
year = {2020},
month = {9}
}

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