Film Thickness and Composition Effects in Symmetric Ternary Block Copolymer/Homopolymer Blend Films: Domain Spacing and Orientation

Toth, Kristof; Bae, Suwon; Osuji, Chinedum O.; Yager, Kevin G.; Doerk, Gregory S.

doi:10.1021/acs.macromol.1c01032

Title: Film Thickness and Composition Effects in Symmetric Ternary Block Copolymer/Homopolymer Blend Films: Domain Spacing and Orientation

Journal Article · Mon Aug 30 00:00:00 EDT 2021 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.1c01032· OSTI ID:1818926

^[1]; Bae, Suwon ^[2];

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Yale Univ., New Haven, CT (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Univ. of Pennsylvania, Philadelphia, PA (United States)

We report thickness and homopolymer molar mass dependencies in thin film blends of a compositionally symmetric 75 kg/mol lamellar polystyrene-block-poly(methyl methacrylate) diblock copolymer (PS-b-PMMA) with near-equal volume fractions of PS and PMMA homopolymers on “neutral” surfaces that promote a vertical domain orientation. PS and PMMA homopolymers with equal molar masses of 1, 3, and 22 kg/mol are blended in a 1:1 mass ratio. To efficiently explore this parameter space, we prepared combinatorial samples with gradient homopolymer concentrations using electrospray deposition (ESD) and gradient film thicknesses using flow coating; these samples were subsequently characterized by grazing-incidence small-angle X-ray scattering and scanning electron microscopy, respectively. Our results demonstrate that the added homopolymers increase or reduce domain spacings with respect to the neat (unblended) block copolymer depending on their molar masses, in line with previous reports; a simple heuristic to estimate the domain scaling in ternary blends based on the homopolymer molar mass agrees well with data for the thinnest blend films studied here. More surprisingly, we observe that the measured domain spacing in blends also depends on film thickness, with thicker films exhibiting larger domain spacings than thinner films at the same homopolymer concentration. Furthermore, thickness gradients at fixed homopolymer concentrations reveal a change in lamellae orientation from vertical to horizontal as film thickness is increased beyond the nominal lamellar domain spacing. Coarse-grained molecular dynamics simulations indicate that this change in orientation is induced by homopolymer segregation to film surfaces. Finally, tying these effects together, we hypothesize that the observed dependence of domain spacing on film thickness is a consequence of changes in the vertical homopolymer composition profile in thicker films during lamellae reorientation and the conformational asymmetry between PMMA and PS segments.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704

OSTI ID:: 1818926

Report Number(s):: BNL-222070-2021-JAAM

Journal Information:: Macromolecules, Vol. 54, Issue 17; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Thickness
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Organic compounds
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Title: Film Thickness and Composition Effects in Symmetric Ternary Block Copolymer/Homopolymer Blend Films: Domain Spacing and Orientation

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