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Title: Chain Conformation near the Buried Interface in Nanoparticle-Stabilized Polymer Thin Films

It is known that when nanoparticles are added to polymer thin films, they often migrate to the film-substrate interface and form an “immobile interfacial layer”, which has been believed as the origin of suppression of dewetting. We here report an alternative mechanism of dewetting suppression from the structural aspect of a polymer. Dodecane thiol-functionalized gold (Au) nanoparticles embedded in PS thin films prepared on Si substrates were used as a model. It was found that thermal annealing promotes irreversible polymer adsorption onto the substrate surface along with the surface migration of the nanoparticles. We also revealed that the surface migration causes additional nanoconfined space for the adsorbed polymer chains. As a result, the self-organization process of the strongly adsorbed polymer chains on the solid surface was so hindered that the chain conformations were randomized and expanded in the film normal direction. Here, the resultant chain conformation allows the interpenetration between free chains and the adsorbed chains, promoting adhesion and hence stabilizing the thin film.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ; ORCiD logo [1] ; ORCiD logo [1] ;  [2] ;  [3] ;  [4] ;  [4] ;  [5] ; ORCiD logo [5] ; ORCiD logo [6]
  1. Stony Brook Univ., Stony Brook, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States); Columbia Univ., New York, NY (United States)
  4. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  5. Kyushu Univ., Fukuoka (Japan)
  6. The Univ. of Akron, Akron, OH (United States)
Publication Date:
Report Number(s):
BNL-203495-2018-JAAM
Journal ID: ISSN 0024-9297
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Macromolecules
Additional Journal Information:
Journal Volume: 50; Journal Issue: 19; Journal ID: ISSN 0024-9297
Publisher:
American Chemical Society
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1434769

Barkley, Deborah A., Jiang, Naisheng, Sen, Mani, Endoh, Maya K., Rudick, Jonathan G., Koga, Tadanori, Zhang, Yugang, Gang, Oleg, Yuan, Guangcui, Satija, Sushil K., Kawaguchi, Daisuke, Tanaka, Keiji, and Karim, Alamgir. Chain Conformation near the Buried Interface in Nanoparticle-Stabilized Polymer Thin Films. United States: N. p., Web. doi:10.1021/acs.macromol.7b01187.
Barkley, Deborah A., Jiang, Naisheng, Sen, Mani, Endoh, Maya K., Rudick, Jonathan G., Koga, Tadanori, Zhang, Yugang, Gang, Oleg, Yuan, Guangcui, Satija, Sushil K., Kawaguchi, Daisuke, Tanaka, Keiji, & Karim, Alamgir. Chain Conformation near the Buried Interface in Nanoparticle-Stabilized Polymer Thin Films. United States. doi:10.1021/acs.macromol.7b01187.
Barkley, Deborah A., Jiang, Naisheng, Sen, Mani, Endoh, Maya K., Rudick, Jonathan G., Koga, Tadanori, Zhang, Yugang, Gang, Oleg, Yuan, Guangcui, Satija, Sushil K., Kawaguchi, Daisuke, Tanaka, Keiji, and Karim, Alamgir. 2017. "Chain Conformation near the Buried Interface in Nanoparticle-Stabilized Polymer Thin Films". United States. doi:10.1021/acs.macromol.7b01187. https://www.osti.gov/servlets/purl/1434769.
@article{osti_1434769,
title = {Chain Conformation near the Buried Interface in Nanoparticle-Stabilized Polymer Thin Films},
author = {Barkley, Deborah A. and Jiang, Naisheng and Sen, Mani and Endoh, Maya K. and Rudick, Jonathan G. and Koga, Tadanori and Zhang, Yugang and Gang, Oleg and Yuan, Guangcui and Satija, Sushil K. and Kawaguchi, Daisuke and Tanaka, Keiji and Karim, Alamgir},
abstractNote = {It is known that when nanoparticles are added to polymer thin films, they often migrate to the film-substrate interface and form an “immobile interfacial layer”, which has been believed as the origin of suppression of dewetting. We here report an alternative mechanism of dewetting suppression from the structural aspect of a polymer. Dodecane thiol-functionalized gold (Au) nanoparticles embedded in PS thin films prepared on Si substrates were used as a model. It was found that thermal annealing promotes irreversible polymer adsorption onto the substrate surface along with the surface migration of the nanoparticles. We also revealed that the surface migration causes additional nanoconfined space for the adsorbed polymer chains. As a result, the self-organization process of the strongly adsorbed polymer chains on the solid surface was so hindered that the chain conformations were randomized and expanded in the film normal direction. Here, the resultant chain conformation allows the interpenetration between free chains and the adsorbed chains, promoting adhesion and hence stabilizing the thin film.},
doi = {10.1021/acs.macromol.7b01187},
journal = {Macromolecules},
number = 19,
volume = 50,
place = {United States},
year = {2017},
month = {9}
}