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Title: Nanoscale Particle Motion Reveals Polymer Mobility Gradient in Nanocomposites

Abstract

Polymer mobility near nanoparticle surfaces has been extensively discussed; however, direct experimental observation in the nanocomposite melts has been a difficult task. Here, by taking advantage of large dynamical asymmetry between the miscible matrix and surface-bound polymers, we highlighted their interphases and studied the resulting effect on the nanoparticle relaxation using X-ray photon correlation spectroscopy. Here, the local mobility gradient is signified by an unprecedented increase in the relaxation time at length scales on the order of polymer radius of gyration. The effect is accompanied by a transition from simple diffusive to subdiffusive behavior in accord with viscous and entangled dynamics of polymers in the matrix and in the interphase, respectively. Our results demonstrate that the nanoparticle-induced polymer mobility changes in the interphases of nanocomposite melts can be extracted from the length-scale-dependent slow particle motion.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]
  1. Koç Univ., Istanbul (Turkey)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. NIST Center for Neutron Research, Gaithersburg, MD (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1559454
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Macro Letters
Additional Journal Information:
Journal Volume: 8; Journal Issue: 5; Journal ID: ISSN 2161-1653
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; nanoparticle dynamics; interface; interphase; polymer nanocomposites; bound polymer

Citation Formats

Senses, Erkan, Narayanan, Suresh, and Faraone, Antonio. Nanoscale Particle Motion Reveals Polymer Mobility Gradient in Nanocomposites. United States: N. p., 2019. Web. doi:10.1021/acsmacrolett.9b00176.
Senses, Erkan, Narayanan, Suresh, & Faraone, Antonio. Nanoscale Particle Motion Reveals Polymer Mobility Gradient in Nanocomposites. United States. doi:10.1021/acsmacrolett.9b00176.
Senses, Erkan, Narayanan, Suresh, and Faraone, Antonio. Wed . "Nanoscale Particle Motion Reveals Polymer Mobility Gradient in Nanocomposites". United States. doi:10.1021/acsmacrolett.9b00176. https://www.osti.gov/servlets/purl/1559454.
@article{osti_1559454,
title = {Nanoscale Particle Motion Reveals Polymer Mobility Gradient in Nanocomposites},
author = {Senses, Erkan and Narayanan, Suresh and Faraone, Antonio},
abstractNote = {Polymer mobility near nanoparticle surfaces has been extensively discussed; however, direct experimental observation in the nanocomposite melts has been a difficult task. Here, by taking advantage of large dynamical asymmetry between the miscible matrix and surface-bound polymers, we highlighted their interphases and studied the resulting effect on the nanoparticle relaxation using X-ray photon correlation spectroscopy. Here, the local mobility gradient is signified by an unprecedented increase in the relaxation time at length scales on the order of polymer radius of gyration. The effect is accompanied by a transition from simple diffusive to subdiffusive behavior in accord with viscous and entangled dynamics of polymers in the matrix and in the interphase, respectively. Our results demonstrate that the nanoparticle-induced polymer mobility changes in the interphases of nanocomposite melts can be extracted from the length-scale-dependent slow particle motion.},
doi = {10.1021/acsmacrolett.9b00176},
journal = {ACS Macro Letters},
issn = {2161-1653},
number = 5,
volume = 8,
place = {United States},
year = {2019},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
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