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    Photoinscription of Chain Anisotropy into Polymer Networks
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    † Department of Chemical Engineering, University of Rochester, Rochester, New York 14627-0166, United States
    ‡ Laboratory of Laser Energetics, University of Rochester, Rochester, New York 14623-1212, United States
    *E-mail [email protected]; tel (585) 273-5526, fax (585) 273-1348 (M.A.).
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    Macromolecules

    Cite this: Macromolecules 2016, 49, 23, 9100–9107
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    https://doi.org/10.1021/acs.macromol.6b01990
    Published November 21, 2016
    Copyright © 2016 American Chemical Society
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    Abstract

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    Fixing chain orientation within polymeric materials can impart anisotropic mechanical, optical, and electrical properties. Although macroscopic anisotropy in amorphous or liquid crystalline phases has been achieved by cross-linking or by thermoreversible bond shuffling under strain, these methods lack spatial and temporal resolution. Here, we demonstrate a method to controllably write chain anisotropy into polymer networks containing both permanent and light-sensitive bonds. While held under mechanical stress or strain, light initiates a cascade of addition–fragmentation chain transfer reactions, causing photosensitive functional groups to reshuffle, thereby stabilizing the deformed network. Photoinscription of chain anisotropy allows for simplified processing on fully cross-linked networks with spatial and temporal control over chain orientation, thus enabling a spectrum of anisotropic polymeric materials. As an example, we demonstrate how built-in anisotropy of a semicrystalline network encourages crystallization along a preferred direction, leading to fully reversible shape actuation.

    Copyright © 2016 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.macromol.6b01990.

    • Calculation of percolation threshold; transient network model with external stress; fitting photoinduced creep data with transient network model; fitting photoinduced stress relaxation with transient network model; analysis of stress–strain behavior following fixed-strain photoprogramming (PDF)

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    Macromolecules

    Cite this: Macromolecules 2016, 49, 23, 9100–9107
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.macromol.6b01990
    Published November 21, 2016
    Copyright © 2016 American Chemical Society
    Request reuse permissions

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