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Title: Exploiting Molecular Weight Distribution Shape to Tune Domain Spacing in Block Copolymer Thin Films

Abstract

We report a method for tuning the domain spacing (Dsp) of self-assembled block copolymer thin films of poly(styrene-block-methyl methacrylate) (PS-b-PMMA) over a large range of lamellar periods. By modifying the molecular weight distribution (MWD) shape (including both the breadth and skew) of the PS block via temporal control of polymer chain initiation in anionic polymerization, we observe increases of up to 41% in Dsp for polymers with the same overall molecular weight (Mn ≈ 125 kg mol–1) without significantly changing the overall morphology or chemical composition of the final material. In conjunction with our experimental efforts, we have utilized concepts from population statistics and least-squares analysis to develop a model for predicting Dsp based on the first three moments of the MWDs. This statistical model reproduces experimental Dsp values with high fidelity (with mean absolute errors of 1.2 nm or 1.8%) and provides novel physical insight into the individual and collective roles played by the MWD moments in determining this property of interest. As a result, this work demonstrates that both MWD breadth and skew have a profound influence over Dsp, thereby providing an experimental and conceptual platform for exploiting MWD shape as a simple and modular handle for fine-tuningmore » Dsp in block copolymer thin films.« less

Authors:
 [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]
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  1. Cornell Univ., Ithaca, NY (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1489032
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 13; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Gentekos, Dillon T., Jia, Junteng, Tirado, Erika S., Barteau, Katherine P., Smilgies, Detlef -M., DiStasio, Jr., Robert A., and Fors, Brett P. Exploiting Molecular Weight Distribution Shape to Tune Domain Spacing in Block Copolymer Thin Films. United States: N. p., 2018. Web. doi:10.1021/jacs.8b00694.
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Gentekos, Dillon T., Jia, Junteng, Tirado, Erika S., Barteau, Katherine P., Smilgies, Detlef -M., DiStasio, Jr., Robert A., & Fors, Brett P. Exploiting Molecular Weight Distribution Shape to Tune Domain Spacing in Block Copolymer Thin Films. United States. https://doi.org/10.1021/jacs.8b00694
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Gentekos, Dillon T., Jia, Junteng, Tirado, Erika S., Barteau, Katherine P., Smilgies, Detlef -M., DiStasio, Jr., Robert A., and Fors, Brett P. Fri . "Exploiting Molecular Weight Distribution Shape to Tune Domain Spacing in Block Copolymer Thin Films". United States. https://doi.org/10.1021/jacs.8b00694. https://www.osti.gov/servlets/purl/1489032.
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@article{osti_1489032,
title = {Exploiting Molecular Weight Distribution Shape to Tune Domain Spacing in Block Copolymer Thin Films},
author = {Gentekos, Dillon T. and Jia, Junteng and Tirado, Erika S. and Barteau, Katherine P. and Smilgies, Detlef -M. and DiStasio, Jr., Robert A. and Fors, Brett P.},
abstractNote = {We report a method for tuning the domain spacing (Dsp) of self-assembled block copolymer thin films of poly(styrene-block-methyl methacrylate) (PS-b-PMMA) over a large range of lamellar periods. By modifying the molecular weight distribution (MWD) shape (including both the breadth and skew) of the PS block via temporal control of polymer chain initiation in anionic polymerization, we observe increases of up to 41% in Dsp for polymers with the same overall molecular weight (Mn ≈ 125 kg mol–1) without significantly changing the overall morphology or chemical composition of the final material. In conjunction with our experimental efforts, we have utilized concepts from population statistics and least-squares analysis to develop a model for predicting Dsp based on the first three moments of the MWDs. This statistical model reproduces experimental Dsp values with high fidelity (with mean absolute errors of 1.2 nm or 1.8%) and provides novel physical insight into the individual and collective roles played by the MWD moments in determining this property of interest. As a result, this work demonstrates that both MWD breadth and skew have a profound influence over Dsp, thereby providing an experimental and conceptual platform for exploiting MWD shape as a simple and modular handle for fine-tuning Dsp in block copolymer thin films.},
doi = {10.1021/jacs.8b00694},
journal = {Journal of the American Chemical Society},
number = 13,
volume = 140,
place = {United States},
year = {2018},
month = {3}
}
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    • DOI: 10.1039/c9sc04736k

    Deconstructing Oligomer Distributions: Discrete Species and Artificial Distributions
    journal, September 2019

    • De Neve, Jeroen; Haven, Joris J.; Harrisson, Simon
    • Angewandte Chemie International Edition, Vol. 58, Issue 39
    • DOI: 10.1002/anie.201906842

    Amphiphilic fluorous random copolymer self‐assembly for encapsulation of a fluorinated agrochemical
    journal, September 2018

    • Ko, Jeong Hoon; Bhattacharya, Arvind; Terashima, Takaya
    • Journal of Polymer Science Part A: Polymer Chemistry, Vol. 57, Issue 3
    • DOI: 10.1002/pola.29187

    Tuning Dispersity by Photoinduced Atom Transfer Radical Polymerisation: Monomodal Distributions with ppm Copper Concentration
    journal, August 2019

    • Whitfield, Richard; Parkatzidis, Kostas; Rolland, Manon
    • Angewandte Chemie, Vol. 131, Issue 38
    • DOI: 10.1002/ange.201906471

    Deconstructing Oligomer Distributions: Discrete Species and Artificial Distributions
    journal, July 2019

    • De Neve, Jeroen; Haven, Joris J.; Harrisson, Simon
    • Angewandte Chemie, Vol. 131, Issue 39
    • DOI: 10.1002/ange.201906842

    Tailoring polymer dispersity and shape of molecular weight distributions: methods and applications
    text, January 2019

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